- Invented the boom microphone.
- He was one of the very few screen actors in the 1930s, 1940s and early 1950s who had a prolific career despite being in a wheelchair. From 1938, his screen roles were written to accommodate his disability.
- He and his sister Ethel Barrymore were the first Oscar-winning brother and sister in acting categories.
- Great uncle of Drew Barrymore.
- Honorary pallbearer at Lon Chaney's funeral.
- Acted from wheelchair from 1938 due to the effects of arthritis and hip injury.
- He played Scrooge in "A Christmas Carol" on the radio annually for 20 years between 1934 and 1953. He missed only twice. In 1936 his brother John replaced him because of the Christmas Eve death of his wife and in 1938 by Reginald Owen, whose MGM version was then in theatrical release.
- Had extreme problems with his income taxes, and during the last 15 years of his life routinely turned over all of his paycheck to the Internal Revenue Service except for a small sum to maintain his living expenses. The IRS also took the proceeds from a sale of his artwork after his death.
- Reared Roman Catholic by their mother, the three Barrymore siblings all had suffered the stigma of divorce (doubtless connected to the family business) and only Ethel Barrymore was a practicing Catholic in adulthood.
- In Rasputin and the Empress (1932), he played Rasputin, allegedly the lover of Czar Nicholas II's wife Alexandra, played by Barrymore's real-life sister Ethel Barrymore. Their brother, John Barrymore played the role of Prince Chegodieff in the same film.
- He appeared in two Best Picture Academy Award winners: Grand Hotel (1932) and You Can't Take It with You (1938). Lee Phelps also appeared in both films.
- Barrymore was a member of the historical actor's club of New York, The Lambs, in 1900 and remained a member until his death.
- He has two stars on the Hollywood Walk of Fame - for motion pictures at 1724 Vine Street and for radio at 1651 Vine Street.
- His name appeared in the Looney Toons Cartoon One Froggy Evening (1955) (directed by Chuck Jones) in a newspaper on a park bench before the distraught man was sent to a psychiatric ward because the frog would not sing in front of anyone else.
- Directed two actors to Oscar nominations: Ruth Chatterton (Best Actress, Madame X (1929), technically not an official nominee), and Lawrence Tibbett (Best Actor, The Rogue Song (1930)).
- Had two daughters with his first wife Doris Rankin, both of whom died young. He later left Rankin for Irene Fenwick, a longtime friend and one-time girlfriend of his brother, John Barrymore.
- The three Barrymore siblings appeared in only one film together: Rasputin and the Empress (1932). Lionel and John appeared without Ethel in Arsène Lupin (1932), Grand Hotel (1932), Night Flight (1933) and Dinner at Eight (1933). A decade after John's demise, Lionel and Ethel appeared in Main Street to Broadway (1953), Lionel's last film.
- Interred at Calvary Cemetery, Los Angeles, California, USA, in the Main Mausoleum, Block 352.
- Started as a stock player at the Biograph Company.
- He was buried a Roman Catholic next to his second wife and his brother, John Barrymore, in Calvary Cemetery, Hollywood.
- He and Spring Byington played husband and wife in Ah Wilderness! (1935). Three years later, they played father and daughter in You Can't Take It with You (1938).
- Spent most of his screen career under contract to MGM (1926-52).
- Portrayed Dr. Gillespie on the syndicated radio show "The Story of Dr. Kildare" (1950-1951), and in the late-1930s/'40s movie series.
- Son of Maurice Barrymore and Georgiana Barrymore; grandson of Louisa Drew and stage actor John Drew (1827-1862); nephew of Sidney Drew; cousin of S. Rankin Drew. Fathered two daughters: Ethel (1909-1910) and Mary (1916-1917).
- Screen, stage, radio, vaudeville actor, film producer, and screenwriter.
- Was just 22 years older than Jean Arthur, who played his granddaughter in You Can't Take It with You (1938).
- Studied musical composition with Eugene Zador for ten years.
- Starred in seven Oscar Best Picture nominees: The Hollywood Revue of 1929 (1929), Grand Hotel (1932), Captains Courageous (1937), Test Pilot (1938), You Can't Take It with You (1938), Since You Went Away (1944) and It's a Wonderful Life (1946). Grand Hotel and You Can't Take It with You won.
- Counting unofficial nominees, is the first person to have Academy Award nominations for Best Actor (for A Free Soul (1931), which he won) and Best Director (for Madame X (1929)).
- In the 1960s cartoon series Underdog (1964), Underdog's nemesis, Simon Bar Sinister, has a voice reminiscent of Barrymore's, though it was actually voiced by Allen Swift.
- He has appeared in four films that have been selected for the National Film Registry by the Library of Congress as being "culturally, historically or aesthetically" significant: Ben-Hur: A Tale of the Christ (1925), Grand Hotel (1932), Dinner at Eight (1933) and It's a Wonderful Life (1946).
- In 1930, he lived at 802 N. Roxbury Drive in Beverly Hills.
- He and his sister Ethel are the only brother and sister Oscar winners.
- In the 1950 census, he is a lodger with Florence R Wheeler, Maryellen Wheeler and Violet Grace Wheeler.
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