Never known as a solo performer (despite the existence of an unsold television pilot called The Arnold Stang Show), he works best in, and prefers, an ensemble cast in which he plays only one of a diverse group of comic characters.

On radio, he was popular in the late 1940s as a sidekick to comedian Henry Morgan. In movies, he played Sparrow in The Man with the Golden Arm (1955) alongside Frank Sinatra and Kim Novak. In It's a Mad, Mad, Mad, Mad World (1963) he played Ray, who along with his partner Irwin (played by Marvin Kaplan) owns a gas station that is destroyed by Jonathan Winters. In one of the weirdest-ever movie pairings, he was teamed with the young Arnold Schwarzenegger (billed as "Arnold Strong") in the latter's first film, the camp classic Hercules in New York (1970). As a voice actor for animated cartoons, he provided the voice for Popeye's pal Shorty, Herman the mouse in a number of Famous Studios cartoons, the Hanna-Barbera character Top Cat and Catfish on Misterjaw. In television commercials, he was spokesman for the Chunky candy bar, when he would (after listing most of the ingredients) smile and say, "Chunky, what a chunk of chocolate!" He provided the voice of the Honey Nut Cheerios Bee in the 1980s and also spoke for Vicks Vapo-Rub. His wife, Joanne Stang, is a writer for the New York Times.