Arberry came up to Pembroke College in 1924. He took firsts in both parts of the Classics tripos. He was awarded one of the newly created Browne studentship and took the Arabic and Persian tripos, where he again gained firsts in both parts. In 1931 he was elected to a research fellowship at Pembroke College. In 1944 he took up the chair of Persian at London University. In 1946 he became professor of Arabic and head of the Near and Middle East department, but in 1947 he left London to return to his old college at Cambridge, as Sir Thomas Adams's professor of Arabic, a post which he held for the remainder of his life.