"Falling in love and religious experiences I've had are often tremendously similar," said Laurel Sprengelmeyer, the Montreal musician known to her fans as Little Scream. "You have this feeling of a huge awakening, and the surge of endorphins. Religion and the cult of love – they're not unrelated."

Sprengelmeyer's experience of the phenomenon may be deeper than most, thanks to her years as an enthusiastic Jehovah's Witness. For her, a love song is almost bound to have a sacred undercurrent, as if finding the One and meeting the one were almost the same thing.

"I think there's a cult in relationships, where we have an idea of what we're interacting with, and it's not the reality," she said, sitting in her bright studio in Montreal's Plateau district. "We subscribe ourselves to an idea of what the relationship is, and then it becomes a cult, which everyone around you confirms socially. It becomes a real thing that has power over your life."

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You can hear the fusion of romance and religion in Cult Following, her new and much-anticipated second album, though not through overt references to anything godly. It's more in the point of view, the atmosphere and the expectation that daily experience can disclose miracles.

"There's something incredibly comforting about having answers for everything," Sprengelmeyer said. She was speaking nostalgically, as someone who quit the church, but can't renounce the experience of order and certainty that came from being part of it.

She felt the lure of those things again, from a greater remove, while visiting a friend at a Brazilian spiritual retreat three years ago. A following had coalesced around a charismatic leader who also seemed to have answers for everything. Sprengelmeyer recognized all the signs of cult devotion, including the unspoken methods for controlling thought and behaviour.

"It was beautiful and hilarious and profound and insane, simultaneously," she said, laughing. It provided the spur for the current record, because she realized she still hadn't worked through the meaning of her time inside that kind of group certainty.

"I had the hilarious misfortune of being born into an evangelical Christian family on my mom's side, and also being converted into it, because my mom got excommunicated when I was 8 or 9," she said. "I was very close to my grandmother, and I wanted to keep the family together, and I became the head of the family from the Jehovah's Witness perspective. I was a real little idealist between the ages of nine and 12."

Her parents split up at around the same time, and set up in different towns on either side of the northern Mississippi River. While her mother's clan in Dubuque, Iowa, weighed its relationship with God, her father presided over a jumble of transitory things in his antique shop in Galena, Ill. "My siblings and I were the dirty little kids at the back of the store," Sprengelmeyer said.

But she also had to be the clean-living acolyte, devoted to the rules of the faith. "You get addicted to a certain restriction, a certain structure," she said, though she can also shudder at how that was enforced. "It was like growing up in a totalitarian society. When you're in that culture, when you see someone straying, it's your responsibility to tell the elders and keep everyone in the flock."

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She was called out before the elders herself, when her jeans were too ragged or her acquaintances too worldly. She wasn't supposed to spend time with those who might lead her away from Scripture. One incident in particular sticks with her, perhaps because it showed the depth of her church's aversion to the secular.

"I always did well in standardized testing," she said, "and I got chosen to go to NASA space camp. I was so excited, but the woman I was studying the Bible with said, 'Laurel, you're going to be hanging out with worldly people, who are going to tell you things that aren't in the Bible. What would Jehovah want you to do?' So of course I didn't go to NASA space camp, and in subsequent years I dropped out of all my honours courses, because the church discouraged education and I wasn't supposed to go to university." She eventually did study studio visual art on a full scholarship at the University of Iowa, following in a long familial line of painters.

All the time she was with the church, her father quietly seeded her consciousness with a more rebellious curriculum. "He was every bohemian child's dream dad," who introduced her to Allen Ginsberg, took her to hear Laurie Anderson and gave her books by Jean Genet and Hunter S. Thompson. She was particularly taken with Genet's ability to find something holy even in a squalid bar or prison cell.

"Genet was one of my favourites, because of the emotional prison I was in," she said. "My romantic world was shaped by that, by the emotional prison of my religious experience. I've never found a compelling reason to give up that perspective, and the transcendence of that romanticism and religiosity. You transform the world through your own consciousness."

Genet also refused to be ashamed of anything, and that too was an inspiration. Sprengelmeyer said she tried several times to remove from the new album sentiments she found too adolescent for a thirtysomething singer-songwriter. But she couldn't drive them out, and took that as a sign that they needed to be relived and re-examined.

"It's this fugue that's created in our youth, and the rest of our lives we spend iterating that in various ways, and transforming it slowly through those iterations. But you also wonder: How long do I have to keep doing this?" she said, with a laugh.

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Working over the same themes and material is a constant part of her practice, as musician and painter. In her studio, several canvases awaited the next phase of their evolution, which can often take four years to complete. Sprengelmeyer has trouble finishing things or letting them go, whichever comes first.

"I think of every song as its own world and its own environment, like a painting," she said. And like a painting, a song can almost always use one more dab of colour. She has spent hours trying to introduce some instrumental effect that may be barely noticeable and lasts only a few seconds.

Music for her is social, she said, in a way that painting isn't. Making songs is a chance to play with others, starting with her creative partner Richard Reed Parry, of Arcade Fire. Others who appear on the album include Mary Margaret O'Hara, Sufjan Stevens, Kyp Malone and Sprengelmeyer's sister Lily, who contributed the groove to the Prince-like party song Love as a Weapon, the album's first video and single.

Some of Sprengelmeyer's current paintings belong to a series of works related to a photo-booth snapshot of an anonymous man, whom she has placed in many different visual environments – another fugue that demands to be worked out. "I'm obsessed with trying to make something with an image that's completely devoid of context, but that can still be meaningful to you, without you having to understand any structure."

Her own peak experience of decontextualization came when she split with the Jehovah's Witnesses. She was immediately ostracized by almost everyone she knew. "I didn't even know how to make friends outside that world," she said.

She met someone whose family had been virtually wiped out during the Rwandan genocide, and while she doesn't at all equate those experiences, the abrupt loss of a personal network drew them together. When he left for Montreal in 2001, she went too, relieved to leave Iowa and the church behind.

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She studied design at Concordia University, painted and continued the nearly private music-making that had begun in Dubuque with informal lessons in guitar and voice from family friends. Her first album, 2011's The Golden Record, was widely praised and long-listed for the Polaris Music Prize in 2011. The response and subsequent touring forced her to polish up her craft as a live performer, and to become more adept at production. She pretty much had to – some of her new songs are mixed from 120 different tracks.

The results are complex and luminous. The pinnacle may be Wishing Well, which is like passing through a series of doors into ever more magical environments. "Open up your wishing well," Sprengelmeyer sings repeatedly, offering an image of hopeful concealment that isn't far from the enclosed spring and sealed fountain of the Bible's Song of Songs. You get the same feeling of open-hearted purity and splendour, embodied in a magnificent panoply of sound.

Sprengelmeyer's religious axis these days runs through Buddhism, which doesn't ask you to believe that dinosaurs appeared before the seventh day. Committing to something appeals to her, she said, because that also means committing to learning about the world and yourself – as she did even as a Jehovah's Witness.

"I feel like I understand the fundamentalism and insanity we see in the world today," she said. "I remember having conversations with people who were studying the Bible with me, saying, 'Laurel, you have to be willing to be sawn asunder before you would renounce your faith.' There was something really awesome about that, about going all the way with it."

Again she laughed, with amusement and wonder at having gotten out alive; but also perhaps because in spite of everything crazy and extreme that came with it, the house of God as she knew it was a beautiful place. There were many rooms there, and sometimes she can still see them in the eyes of another.

Little Scream plays Montreal's Fairmount Theatre on May 11 and Lee's Palace in Toronto on May 12. Cult Following, her new album on Dine Alone Records, was released on May 6.