Bunn was appointed stage manager of Drury Lane Theatre, London, in the year 1823. In 1826, he was managing the Theatre Royal in Birmingham, and in 1833 he undertook the joint management of Drury Lane and Covent Garden, London. In this undertaking he met with vigorous opposition. A bill for the abolition of the patent theatres was passed in the House of Commons, but on Bunn's petition was thrown out by the House of Lords. He had difficulties first with his company, then with the lord chamberlain, and had to face the keen rivalry of the other theatres.
A longstanding quarrel with William Charles Macready resulted in the tragedian assaulting the manager. In Macready's own words, he walked past Bunn's door and “going up to him as he sat on the other side of the table, I struck him as he rose a backhanded slap across the face. I did not hear what he said, but I dug my fist into him as effectively as I could; he caught hold of me, and got at one time the little finger of my left hand in his mouth, and bit it.”
Bunn also quarreled with the opera singer Jenny Lind, the "Swedish Nightingale", over her contract. According to Lind's biographers, Henry Scott Holland and W. S. Rockstro, the singer “was so terrified at the penalties, the law-suits, and the disgrace with which Mrs. Bunn had threatened her, that her dearest and most trusted friends could not persuade her to entertain the idea of appearing at an English theatre, under any circumstances, or upon any terms whatever." The controversy was recorded by Bunn in his The Case of Bunn Versus Lind.
Artistically, his control of his English theatres was highly successful. Nearly every leading English actor of the time played under his management, and he made an attempt to establish English opera, producing the principal works of Michael William Balfe. He had some gift for writing, and most of the libretti of these operas were translated by him. In The Stage Before and Behind the Curtain (3 vols., 1840), he gave a full account of his managerial experiences.
In James Joyce's Ulysses, the main character Leopold Bloom thinks briefly (and incompletely) of a lyric Bunn wrote: "Whose smile upon each feature plays with such and such replete”. The original lyric, from the William Vincent Wallace opera Maritana, is: “Whose smile upon each feature plays with truthfulness replete".
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- One or more of the preceding sentences incorporates text from a publication now in the public domain: Chisholm, Hugh, ed. (1911). "Bunn, Alfred". Encyclopædia Britannica. 4 (11th ed.). Cambridge University Press. p. 799.
- Macready, William Charles (1912). The Diaries of William Charles Macready, 1833-1851. New York: G. P. Putnam’s Sons. p. 380.
- Holland, Henry Scott (1891). Memoir of Madame Jenny Lind-Goldschmidt. London: John Murray. p. 429.