He served in the U.S. Army Air Forces' First Motion Picture Unit making training films during World War II.
Albertson made well over one hundred appearances (1923–1964) in movies and television. In his early career he often sang and danced in such films as Just Imagine (1930) and A Connecticut Yankee (1931). He was featured in Alice Adams (1935) as the title character's brother, and in Room Service (1938) he played opposite the Marx Brothers. As he aged he moved from featured roles to supporting and character parts—in his later career he can be seen as Sam Wainwright, the businessman fond of saying "Hee-Haw" in the movie It's a Wonderful Life (1946).
Albertson portrayed future U.S. President Theodore Roosevelt in the 1956 episode "Rough Rider" of the CBS western television series,My Friend Flicka. He guest starred in the early NBC western series, The Californians and twice in the David Janssen crime drama,Richard Diamond, Private Detective.
He was cast in 1959 and 1962 in different roles on Walter Brennan's sitcom, The Real McCoys. In 1960, He appeared as General Devery in the episode "Strange Encounter" of the ABC/Warner Brothers western series Colt .45.
In 1960, he played the wealthy rancher, Tom Cassidy, at the beginning of Psycho (1960), who provides the $40,000 in cash that Janet Leigh's character later steals. In the 1960-1961 television season, he played the character Mr. Cooper in five episodes of the CBSsitcom, Bringing Up Buddy, starring Frank Aletter. In 1964, Albertson was cast as Jim O'Neal in the episode "The Death of a Teacher" of the NBC education drama, Mr. Novak.
One of his final screen appearances was as "Sam," the bewildered mayor of Sweet Apple, Ohio, in the 1963 musical Bye Bye Birdie.
Albertson died in his sleep at his home in Santa Monica, California. He was survived by his wife Grace and four children.
For contributions to the motion picture industry, Frank Albertson was honored with a star on the Hollywood Walk of Fame at 6758 Hollywood Boulevard.