June Foray in 1967. She played babies and birds and sexy dames, along with doting grandmas and cackling witches. (George Brich/Associated Press)

June Foray, a voice actress who portrayed croaky grandmothers, purring cats and the world’s most famous flying rodent — Rocket J. Squirrel, from “The Rocky and Bullwinkle Show” — in hundreds of animated movies, television series and commercials, died July 26 at a Los Angeles hospital. She was 99.

Her niece, Robin Thaler, said the cause was cardiac arrest.

Few actors — or everyday, ­performance-averse human beings, for that matter — maintained as much control over their voice as Ms. Foray, who received a star on the Hollywood Walk of Fame in 2010 and an honorary Emmy Award three years later.

She portrayed elderly women even as a child, going on the radio at 12 with the help of an acting teacher. In 2014, as a very senior citizen, she played the Looney Tunes role of Granny, owner of Sylvester the Cat and Tweety Bird, with the same good-

natured screeches and yawlps she used for the character a half- century earlier.

Ms. Foray sometimes drew comparisons to the actor Lon Chaney, known as the silent film era’s “man of a thousand faces” because of his ability to inhabit many roles. She was also placed in a virtuosic league of her Looney Tunes colleague Mel Blanc, who gave voice to Bugs Bunny — whom Ms. Foray pursued as the sinister Witch Hazel — and Daffy Duck and a host of other characters.

Ms. Foray played characters such as Granny, the owner of Sylvester the Cat and Tweety Bird. (Kevin Winter/Getty Images)

But the comparisons seemed to understate Ms. Foray’s singular position as perhaps the most prolific and dynamic voice actress in Hollywood, capable of conjuring a flesh-and-blood (or fur-and-blood) character using little more than an off-the-cuff drawing or suggestion from a producer.

“June Foray is not the female Mel Blanc,” the legendary animator Chuck Jones once said. “Mel Blanc was the male June Foray.”

Ms. Foray, who stood less than 5 feet tall, played a number of diminutive characters, including Jokey Smurf on “The Smurfs” television series, cheery grandmas (among them Grandmother Fa, bearer of a lucky cricket in the 1998 Disney film “Mulan”) and sweet young children.

She was the voice of Mattel’s pull-string Chatty Cathy doll in the 1960s — and used a similarly friendly tone as Talky Tina, a murderous doll that springs to life in a 1963 episode of “The Twilight Zone.” Three years later, she made one of her most memorable performances as Cindy Lou Who, “who was no more than two,” in Jones’s hit television adaptation of the Dr. Seuss book “How the Grinch Stole Christmas!”

Yet it was her work on “Rocky and Bullwinkle,” which debuted in 1959 on ABC under the name “Rocky and His Friends,” that launched Ms. Foray to enduring acclaim. The brainchild of producer Jay Ward, cartoonist Alex Anderson and head writer Bill Scott, the program was an occasionally surreal sendup of Cold War politics, U.S. variety shows and classic fairy tales.

Ms. Foray initially thought that a program centered on a moose and squirrel was, at best, “a real cockeyed idea.” But the program became a hit, in part because of her portrayal of Rocky — “an all-American squirrel,” Ms. Foray said, who employed the catchphrase “hokey smokes” and seemed to possess the moral compass of a Boy Scout — and of the heavily accented Natasha ­Fatale. The vaguely Russian-sounding archnemesis of Rocky and Bullwinkle was aligned with her “dollink” henchman, Boris Badenov, and a one-eyed mastermind named Fearless Leader.

Ms. Foray also provided the voice for red-haired Nell Fenwick, the love interest of Canadian Mountie Dudley Do-Right. (Nell was more interested in Dudley’s horse, Horse, than in the man.) Rocky and Bullwinkle ran, under several names, until 1964, first on ABC and later on NBC.

Actors John Cho, left, and Kal Penn, right, flank voice artist June Foray as she accepts the Comic-Con Icon award at the 2011 Scream Awards. (Chris Pizzello/AP)

Ms. Foray reprised the role of Rocky for the 2000 combined live-action and animated film “The Adventures of Rocky and Bullwinkle,” a box-office bomb that featured Rene Russo as ­Natasha.

“Everybody loves Rocky,” Ms. Foray told the Associated Press that year, wearing a golden Rocky pendant on her neck. “People don’t think of him as a squirrel. They think of him as a person. And he’s a good little person.”

She was born June Lucille Forer in Springfield, Mass., on Sept. 18, 1917. Her engineer father was a Jewish immigrant from Russia. The family moved to California when she was a teenager.

She recorded children’s albums for Capitol Records in the 1940s and broke through in the following decade spoofing the popular detective series “Dragnet” with comedian Stan Freberg. Her early work also included portraying Lucifer the cat in the 1950 Disney film “Cinderella.”

Her first marriage, to Bernard Barondess, ended in divorce. Her second husband, screenwriter Hobart Donavan, died in 1976. There are no immediate survivors.

In addition to her voice acting, Ms. Foray was a forceful advocate of animation as a medium. She helped build ASIFA-Hollywood, a branch of the International Animated Film Society, and in 1972 created the Annie Awards, an animation-only alternative to the Oscars and Emmys.

As a longtime member of the Academy Awards’ board of governors, she also successfully fought to create an Oscar for best animated feature film. It has been awarded each year since 2002, when it went to the computer-animated comedy “Shrek.”

By then, Ms. Foray had been perhaps too successful in advocating for animation. In “Shrek,” she and her voice-actor peers were supplanted by A-list celebrities — Mike Myers, Eddie Murphy, Cameron Diaz and John Lithgow — who had little experience in the medium.

“We are all doing supplementary parts while Cameron Diaz is getting paid $10 million,” Ms. Foray told the Los Angeles Daily News. “The stars receive millions of dollars for doing voices for animated film and then there is the poor actor who has to struggle to make at least $15,000 a year just to keep his benefits. A lot of the young people — wonderful, good, solid voice actors — have families and are buying homes, and work is bad for them.”