He voiced the Mad Hatter in Alice in Wonderland (1951) and portrayed Uncle Albert in Mary Poppins (1964). He also played as Mr. Toymaker in Babes in Toyland, Fire chief in The Absent-Minded Professor, A. J. Allen in Son of Flubber, Mr. Hofstedder the Jeweler in That Darn Cat!, and (his final role) Rufus the Gnome King in The Gnome-Mobile. In 1933, he was caricatured by Joe Grant in the Mickey Mouse short, Mickey's Gala Premiere.
Wynn died June 19, 1966 in Beverly Hills, California of throat cancer, aged 79. He was interred at Forest Lawn Memorial Park in Glendale, and his gravestone reads "Dear God, Thanks... Ed Wynn".
- His granddaughter stated in her speech when accepting his Disney Legends award on his behalf that Walt Disney was a pallbearer at his funeral.
- His performance as the Mad Hatter served as inspiration and reference for the character King Candy in the 2012 Disney animated film Wreck-It Ralph.
- He was one of the actors approached to play The Wizard in the 1939 classic film, The Wizard Of Oz, however the role was too small for him.
- Chameleon was seen transforming into Ed Wynn in the Mighty Ducks episode; "Beak to the Future".
- His stage name is a pun of his middle name "Edwin".