His other roles include Grandpa Joe in Willy Wonka & the Chocolate Factory (1971), Manny Rosen in The Poseidon Adventure (1972), and Ed Brown in the television sitcom Chico and the Man (1974–1978), for which he won an Emmy.

His sister Mabel taught him the first "time steps" in tap dancing, and he picked up additional routines by watching vaudeville acts that played his hometown.

Around this time, he started singing with a group called "The Golden Rule Four," who held their practice sessions beneath a railroad bridge.

[7] Besides vaudeville and burlesque, he appeared on the stage in many Broadway plays and musicals, including High Button Shoes, Top Banana, The Cradle Will Rock, Make Mine Manhattan, Show Boat, Boy Meets Girl, Girl Crazy, Meet the People, The Sunshine Boys – for which he received a Tony Award nomination for Best Actor, and The Subject Was Roses – for which he won a Tony for Best Supporting Actor.

He had an early minor role in Miracle on 34th Street as a postal worker who redirects dead letters addressed to "Santa Claus" to the courthouse where Kris Kringle is on trial.

Also nominated was Albertson's later Willy Wonka & the Chocolate Factory co-star Gene Wilder, for his role in The Producers.

On January 2, 1961, Albertson was cast as Sampson J. Binton, with DeForest Kelley as Alex Jeffords, in "Listen to the Nightingale", the series finale of Riverboat, starring Darren McGavin.

[12][better source needed] Albertson had a recurring role as the neighbor Walter Burton in eight episodes of the 1962 ABC sitcom Room for One More, with Andrew Duggan and Peggy McCay.

[14] In a 1967 episode of The Andy Griffith Show, he played the ne'er-do-well cousin, Bradford J. Taylor, of series character Aunt Bee (Frances Bavier).

His final theatrical role was as the hunter, Amos Slade, in Disney's 24th animated feature, The Fox and the Hound, originally released in the summer of 1981, four months before his death.

[16] On the morning of November 25, 1981, Albertson died at his Los Angeles home in the Hollywood Hills[15] at the age of 74 from colon cancer.

[8] He and his elder sister, Bewitched actress Mabel Albertson (who died 10 months later from Alzheimer's disease), were cremated and their ashes were scattered in the Pacific Ocean.