Broadway and West End, 1924–1939
Charlot revised A to Z for the Broadway stage as André Charlot's Revue of 1924, which opened at the Times Square Theatre in January of that year. Buchanan co-starred with Lawrence and Beatrice Lillie, and according to his biographer Andrew Lister, the show introduced the American public to "the distinctive charms of the intimate revue" as opposed to the Ziegfeld spectaculars. In December 1924 Buchanan played Lord Algernon Kenilworth in Boodle, in a pre-London try-out in Birmingham and then in the West End. In this piece, described by The Stage as "something more than a musical play ... in parts, really excellent farce", Buchanan's character was obliged to disguise himself as a clown and later as a barmaid: a reviewer in the Birmingham Daily Gazette commented, "Ah! if all barmaids were half as interesting, the whole country would take to drink". His leading lady in this production was June, but in a subsidiary role was Elsie Randolph, who became Buchanan's best-known stage partner in later productions. Despite good notices, the piece had a modest run of 94 performances.
Buchanan appeared in five British films made in 1924–25: The Audacious Mr Squire, The Happy Ending, Settled Out of Court, A Typical Budget and
Bulldog Drummond's Third Round, and returning to stage revue he appeared, co-starring with Lawrence, in Charlot's 1925 production at the Prince of Wales's. He starred in, choreographed and directed an American production of the show at the Selwyn Theatre, New York. It included one of his most celebrated sketches, "The Fox Has Left His Lair", in which he portrayed a last-minute substitute to a male-voice quartet, who is frantically attempting to keep up with his fellow singers in a hunting song that gets faster and faster and ever more complicated. On his return to London he appeared at the Hippodrome in October 1926, when he produced Jerome Kern and Oscar Hammerstein's Sunny, which ran for 363 performances. Buchanan played Jim Demming, with Binnie Hale as Sunny and Elsie Randolph as Weenie Winters. He interpolated the hunting song sketch into the production. At the same theatre in June 1928, after a pre-London tour, he produced That's a Good Girl, in which he appeared as Bill Barrow with Randolph now in the leading female role. Their duet, "Fancy Our Meeting", was recorded by Columbia and became well known. In his 1978 biography of Buchanan, Michael Marshall comments, "this haunting tune is played and sung whenever Jack and Elsie's long partnership is recalled". In the words of Buchanan's biographer Andrew Spicer:
After this, Buchanan's West End and Broadway appearances were mainly in revue and musicals. In his entry in Who's Who he singled out That's a Good Girl (1928), Stand Up and Sing (1931), Mr Whittington (1933) and This'll Make You Whistle (1935) among his inter-war productions in the West End. In all these he was partnered by Randolph. He appeared on Broadway again in 1929 in C. B. Cochran's revue Wake Up and Dream, heading a cast that contained Tilly Losch and Jessie Matthews. "Fancy Our Meeting" was interpolated from There's a Good Girl, and as Buchanan and Matthews did not get on well, this affectionate duet cost them both some effort. Buchanan starred in two early Hollywood talkies, Cole Porter's Paris (1929), with Irene Bordoni, and Monte Carlo (1930) directed by Ernst Lubitsch.
In 1932 Buchanan accepted an invitation to star in George and Ira Gershwin's Pardon My English in the US. When the production opened it was plain to audiences that he was uncomfortable in his dual role as an English aristocrat and a German gangster. At considerable personal expense he bought himself out of his contract and left the cast. The show closed soon afterwards and he did not return to Broadway for six years. His last Broadway show before the Second World War was Howard Dietz and Arthur Schwartz's Between the Devil (1938), with Evelyn Laye and Adele Dixon, in which he played an inadvertent bigamist.
Buchanan starred in several British films during the 1930s. Some were straightforward adaptations of his stage successes, including That's a Good Girl (1933) and This'll Make You Whistle (1936) for Herbert Wilcox's British and Dominions Imperial Studios. Goodnight Vienna (1932), in which he starred opposite Anna Neagle, was based on a BBC-commissioned radio operetta. The Times remarked on how hauntingly Buchanan sang George Posford's songs for the piece. Spicer comments that films more in keeping with Buchanan's image as "the affable playboy" were Brewster's Millions and Come Out of the Pantry (both 1935). The latter includes one of Buchanan's best-known songs, "Everything Stops for Tea".