His first professional job was in a touring production in Germany of Molière's Les Fourberies de Scapin.
In 1948, he began his career in the theatre with Robert Dhéry in Les Branquignols. His first film was Ah! Les belles bacchantes, starring Robert Dhéry, Colette Brosset (Dhéry's then-wife), and Louis de Funès; directed by Jean Loubignac in 1954. Serrault played in the 1955 suspense thriller Les diaboliques, starring Simone Signoret and directed by Henri-Georges Clouzot.
From February 1973 through 1978, he portrayed the role of Albin/Zaza opposite Jean Poiret in the play La cage aux folles, written by Poiret. He recreated the role for the film version of the play, which was released in 1978.

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