Those already acquainted with the young oeuvre of Benny and Josh Safdie — the multitasking fraternal auteur duo with a joint eye to the social fringes of New York City — may see the title of their third narrative feature as a kind of perverse in-joke. “Good Time” is not the first term you’d use to describe “Daddy Longlegs” or “Heaven Knows What,” two sensitive but skin-prickling studies in human breakage; nor does it entirely apply to this nerve-raddling heist-within-a-heist thriller, which merges the Safdies’ signature gutter realism with tight genre mechanics to discomfiting but exhilarating effect.

A career-peak performance from Robert Pattinson, as a scuzzy Queens bank robber on a grimly spiraling mission to break his mentally handicapped brother out of jail, will attract more eyeballs to this A24 release than the rest of the Safdies’ oeuvre combined, though this “Good Time” is still no commercial picnic. Rather, it’s exciting proof of its makers’ ability to chafe and challenge audiences in a growing range of registers.

Even before the knowingly retro typography of the opening titles kicks in, it’s clear that the sweaty urgency of 1970s New Hollywood — in particular, such hard-headed urban dramas as “Dog Day Afternoon” and “Taxi Driver” — is a key point of reference for the Safdies here. Still, if there’s a grainy classicism to the film’s craft, balancing the fevered formal poetry of 2014’s heroin love story “Heaven Knows What” with Lumet-channeling tautness, it’s no simple throwback exercise. “Good Time’s” passing but pointed glimpses of social disenfranchisement across a range of demographics place its narrative squarely in Donald Trump’s America of 2017.

We never learn the exact circumstances that have driven Connie Nikas (Pattinson) and his vulnerable younger brother Nick (Benny Safdie, directing himself for the first time) to the underworld, though the close-shaved script — by Josh Safdie and Ronald Bronstein — deftly alludes to parental absence and familial abuse. Nick, who has unspecified learning disabilities, is less able than his protective older brother to mask his psychological scarring.

“Good Time” opens on an extended therapy session between him and a court-appointed psychiatrist (Peter Verby), which is just beginning to needle at some nervy revelations when Connie breaks it up. It’s a riveting, disorienting intro, placing focus on a less prominent character whose emotional needs nonetheless drive the entire, life-in-the-day narrative. Revealing hitherto unsuspected range and delicacy as a performer, the younger Safdie articulates compacted years of damage and frailty in his short, shambling responses.

Pattinson, by contrast, enters proceedings as a frenzied human cyclone of bad hair and worse decisions. It’s not so much the matted, cheaply peroxided mop and faux diamond earrings that banish the erstwhile “Twilight” star’s willowy brooding from memory: It’s the antic, stressful body language, the rapid, hungry gait of a man with more to run from than run to, that makes Connie sympathetic and repulsive in equal, sometimes simultaneous, measure.

Busting Nick out of institutional confinement to rope him immediately into an elaborately conceived bank robbery nonetheless plagued with rookie errors, Connie is plainly a toxic influence, yet the brothers’ us-against-the-world kinship is palpable — compounded by ace cinematographer Sean Price Williams’ affinity for tight, sea-sick closeups. As in last year’s Cannes breakout “Hell or High Water” (of which “Good Times” plays as a particularly Hadean variation), the crime story here is a pretext to a more searching examination of dysfunctional fraternal love.

It’s some dazzling pretext, though. The onscreen brothers may execute their job in careless haste, but the Safdies thrust us into the heist’s reckless, twisty fallout with glistening pop vigor, occasionally saturating the screen in electric waves of magenta and turquoise, while experimental musician Oneohtrix Point Never’s furious electro-rock score settles sharply between the temples. (It works in brilliant tandem with the film’s throbbing-to-buzzing sound design, for which the younger Safdie can take yet more multi-hyphenate credit.) After an escape attempt that lands Nick back in the grasp of the authorities, Connie’s equally botched mission to retrieve him plays as a kind of waking nightmare, enlivened equally by these surreal formal flourishes and ragged details of everyday humanity.

No secondary characterization is wasted between the hospitals, backlots and hard-up households that Connie passes through on his long night’s journey into day — whether it’s an incandescently wasted Jennifer Jason Leigh as his self-oriented sometime girlfriend Corey, or Taliah Webster, a terrifically unaffected newcomer, as Crystal, a coolly curious but guileless African-American teen drawn into the chaos for want of anything better to do.

Webster’s scenes with Pattinson are at once among the film’s most unsettling and most warmly observational, tacitly noting the social prejudices that unite and divide them both: They may both exist on society’s deprived margins, but it’s the innocent girl’s race that, at one key point, makes her a greater object of the police suspicion than the at-large bank robber beside her. Less subtly, “Good Time” alludes to authoritarian abuse of power when Connie and Crystal channel-flip past one of those gussied-up cop reality shows: “I don’t wanna see them justify this shit,” he mumbles.

The balance of moral crookedness and conscience in “Good Time” is thus a complex one. That the film works such social and psychological nuance into what otherwise amounts to a breathless, battering pulp thriller — precision-edited to 100 minutes, though it feels shorter and antsier still — is perhaps the most impressive of its achievements. These restlessly independent auteurs have passed the genre-foray test with flying neon colors, at no cost or compromise to their abrasively humane worldview. If you’re going to have a good time in a Safdie brothers film, in other words, it’s got to be on their tense, troubled terms.