- Won an Emmy Award for the TV series The Odd Couple (1970) after the show had been canceled. At his acceptance speech, he said, "Thank you. Now, if I only had a job.".
- Appeared on Late Show with David Letterman (1993) a record 70 times.
- He contracted pneumonia following heart bypass surgery in December 2003, and remained hospitalized until his death.
- Was asked in the 1970s if there had been anyone in his career whom he had really disliked. After saying he hated to criticize the dead, he revealed that he had animosity against the late Ethel Barrymore. As a young actor, Randall had appeared in a play with her, and he was offended by her imperious manner, which included a demand that her fellow actors observe absolute silence in the vicinity of her dressing room.
- Suffered from tinnitus, a chronic ringing in the ears. In 1996, he and Jerry Stiller appeared in a public service announcement for the American Tinnitus Association, encouraging viewers to seek diagnosis and treatment.
- He and Jack Klugman performed together in The Pirate's House (1955) from "The Golden Age of Television" period 15 years before they did the classic The Odd Couple (1970).
- First child, Julia Laurette Randall, was born on 11 April 1997; she was named after his mother Julia and actress Laurette Taylor, whom Randall said was "the best actress I've ever seen in my life", and second child, Jefferson Salvini Randall, was born on June 15, 1998; he was named for comedic actor Joseph Jefferson and Italian tragic actor Tommasso Salvini.
- Studied voice for 32 years but did not act on it, quipping, "I have a nice healthy tone, but it's not terribly musical. If beautiful voices are golden, mine is aluminum.".
- Met his wife Heather in a play in New York. She was 50 years his junior.
- He was originally cast as the voice of "Templeton the Rat" in the movie Charlotte's Web (1973) without an audition. When Joseph Barbera realized he wasn't right for the voice, they paid him and hired Paul Lynde instead.
- The son of Moescha Rosenberg, an art dealer, and Julia (nee Finston) Rosenberg, Randall had a sister, Edna, for whom the daughter of Randall's best known character, Felix Unger on The Odd Couple (1970), was named.
- Took ballet classes and danced at a semi-professional level.
- Served as a cryptologist during World War II.
- He has appeared in two films that have been selected for the National Film Registry by the Library of Congress as being "culturally, historically or aesthetically" significant: Will Success Spoil Rock Hunter? (1957) and Pillow Talk (1959).
- He didn't become a parent until the age of seventy-seven.
- Randall graduated from Tulsa Central High School but dropped out of Northwestern University in Illinois, majoring in speech and drama, in order to study acting with Sanford Meisner and dancer Martha Graham at the Neighborhood Playhouse in New York, under the direction of legendary acting coach Sanford Meisner. Later, he was awarded a Doctor of Humane Letters degree in 2002 from Pace University.
- In an effort to bring back classic theater to Broadway, he founded and was artistic director of the nonprofit National Actors Theatre in 1991, using $1 million of his own money and $2 million from corporations and foundations.
- Avid collector of modern art, opera recordings, and antiques.
- He acted in three Broadway shows during the run of Mister Peepers (1952), working on the show on Tuesdays through its Sunday telecast (Broadway shows at the time were dark on Sundays). At one point he worked for 365 consecutive days without a taking a day off.
- A member, from 1972 onward, of the Metropolitan Opera Association, Randall was also National Chairman of the Myasthenia Gravis Foundation, an incurable neuromuscular disease.
- Was nominated for Broadway's Tony Award five times: as Best Actor (Musical) in 1958 for "Oh, Captain!" and, later, as co-producer with his National Actors' Theater of four nominated plays: as Best Revival, in 1993 for "St. Joan" and as Best Revival (Play) in 1994 for "Timon of Athens"; in 1996 for "Inherit the Wind" and in 1997 for "The Gin Game.".
- Reportedly liked to play Yahtzee, but his quirk was on every turn he played specifically for each score opportunity in exact order as it was on the score card (from top to bottom of the left column starting with "Aces", then from top to bottom of the right column, ending with "Yahtzee" or "random").
- Originated the role of E.K. Hornbeck in the Broadway production of "Inherit the Wind," which ran for 806 performances from April 21, 1955, to June 22, 1957, at the National Theater (now the Nederlander Theater). He was still working on his Mister Peepers (1952) series at the beginning of the run of show, filming episodes on Sundays when the theater was dark. His role was played by Gene Kelly in the 1960 film Inherit the Wind (1960). In 1996, his National Actors' Theater company put on a Broadway revival of "Inherit the Wind" that ran for 45 appearances. He was a stand-in for both Anthony Heald as E.K. Hornbeck and George C. Scott as Henry Drummond, taking over the latter role when Scott had to leave the play. Scott was nominated for a 1996 Tony Award for Best Actor in a Play for the role.
- Randall appeared in both the 1954 stage version of Edward Chodorov's "Oh, Men! Oh, Women! as well as the 1957 screen adaptation but in different roles.
- On August 26, 2021, he was honored with a day of his filmography during the Turner Classic Movies Summer Under the Stars.
- A liberal Democrat, in September 2003 he joked in a speech that President George W. Bush and Vice President Dick Cheney would be turned away if they tried to attend his funeral.
- He recalled the making of 7 Faces of Dr. Lao (1964) in an interview in the book "A Sci-Fi Swarm and Horror Horde" (McFarland & Co., 2010) by Tom Weaver.
- Biography in "The Scribner Encyclopedia of American Lives," Volume 7, 2003-2005, pp. 444-446. Farmington Hills, MI: Thomson Gale, 2007.
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