- He was also a teacher, leading workshops in improvisation. Students found him warm, insightful, and very, very funny.
- One of only six actors to receive an Academy Award nomination for Best Actor for his first screen appearance. The other five actors are: Orson Welles, Lawrence Tibbett, James Dean, Paul Muni and Montgomery Clift.
- Although he usually played quirky, fatherly types in his later years, back in the '60s and '70s he was known as an edgy, intense actor. His darkest role is almost certainly Harry Roat in Wait Until Dark (1967), who was a vicious but intelligent psychopath who terrifies a seemingly defenseless blind woman (Audrey Hepburn).
- Disliked filming the scene in Wait Until Dark (1967) where his character Harry Roat Jr terrorizes Suzy Hendrix (Audrey Hepburn).
- A founding member of the folk group The Tarriers, he co-wrote "The Banana Boat Song" (also known as "Day-o"), which later became a mega-hit for Harry Belafonte.
- Founding member, Second City improv troupe.
- In the foreword for the Second City book, Arkin revealed that he was reluctant to head to Chicago. He says that his first paying job as an actor was in St. Louis, where he ran into a fellow who was starting up the Second City theater troupe in Chicago, and said that if Arkin were ever to come to Chicago, he would hire him. Arkin halfheartedly agreed, thinking that it was just a joke, and headed back to New York for another year as a struggling actor. Arkin called the man and asked if a position was still open. The man confirmed it and Arkin headed to Chicago, thinking that his life was over. But when he joined Second City, he said that he realized he was with a group of people who fostered the kind of acting that he was involved in, and protected him from the fear of the world.
- Disowned his involvement in the film Freebie and the Bean (1974), saying he had only accepted the role because, "I needed the bread".
- Two of his movies, Popi (1969) and Freebie and the Bean (1974), were later adapted into television series starring Hector Elizondo in the roles Arkin brought to the screen. Elizondo also co-starred in the television series Chicago Hope (1994) with Arkin's son, Adam Arkin.
- Won Broadway's 1963 Tony Award as Best Featured Actor in a Play for Enter Laughing (1967), for which he also won a Theatre World Award. Ten years later, he was nominated for a 1973 Tony Award as Best Director (Dramatic) for The Sunshine Boys.
- In his later years, he lived in New Mexico with his wife, Suzanne Newlander Arkin.
- He was awarded a Star on the Hollywood Walk of Fame at 6914 Hollywood Boulevard in Hollywood, California on June 7, 2019.
- The longest he went without an Oscar nomination was 38 years, between The Heart Is a Lonely Hunter (1968) and Little Miss Sunshine (2006).
- Was cast in the title role of Inspector Clouseau (1968) after Peter Sellers declined to reprise the role a third time. It was the last Clouseau film until Sellers returned to the role in The Return of the Pink Panther (1975).
- He was originally slated to play Saul Bloom in Steven Soderbergh's Ocean's Eleven (2001); after dropping out of the production, he was replaced by Carl Reiner. Arkin won a 1963 Tony Award as Best Featured Actor in a Play as well as a Theatre World Award playing a character based on Carl Reiner in the Broadway production of Reiner's autobiographical novel Enter Laughing (1967).
- He has appeared in three films that were nominated for the Best Picture Oscar: The Russians Are Coming the Russians Are Coming (1966), Little Miss Sunshine (2006) and Argo (2012), with the latter winning in the category. He gave Oscar nominated performances in all three films, winning Best Supporting Actor for Little Miss Sunshine.
- Was cast in the role of Judge Myron Kovitsky in The Bonfire of the Vanities (1990) when, initially, the producers couldn't pay a million dollars to Walter Matthau, the original choice for the role. When they reached an agreement, Matthau suddenly dropped out and Arkin was cast, to later on be paid $150,000. However, his character was rewritten from a Jewish magistrate to an African-American judge, played by Morgan Freeman.
- Is the only actor to have played Inspector Clouseau who has won a competitive Oscar (Steve Martin won an honorary Oscar).
- Nominated for the 2019 Golden Globe Award in the Best Performance by an Actor in a Supporting Role in a Series, Limited Series or Motion Picture Made for Television category for his role as Norman in The Kominsky Method (2018), but lost to Ben Whishaw for A Very English Scandal (2018).
- Biography in: "Who's Who in Comedy" by Ronald L. Smith. pg. 24-25. New York: Facts on File, 1992. ISBN 0816023387.
- Wrote "The Lemming Condition," "Cassie Loves Beethoven" and "One Present for Flekman's."
- Father-in-law of Phyllis Lyons and Amelia Campbell.
- Grandfather of son Adam Arkin's daughter Molly.
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