During the next five years, Noyes published five additional volumes of poetry, including Poems (1904). One of Noyes' most ambitious works,  Drake: An English Epic, was first published in 1906. The twelve-book, two hundred page epic is thought to be too long by some critics, but nonetheless, an impressive example of Noyes' talent and creativity. Arguably Noyes' most beloved poem,  The highwayman, was published in Forty singing seamen and other poems in 1907.

He married his first wife, Garnett Daniels, in 1907 and spent time between the United States and Great Britain. Noyes' popularity continued to increase as he published more volumes of poetry. By 1914, he was serving as Professor of Modern English Literature at Princeton University.

After the death of his wife in 1926, Noyes converted to Roman Catholicism and married his second wife, Mary Angela Mayne Weld-Blundell. In 1929, the family moved to Lisle Combe, St Lawrence, Isle of Wight where Noyes continued to write essays and poems, culminating in the collection, Orchard's Bay (1939).

Noyes spent much of the Second World War in North America, returning to Great Britain in 1949. Two world's for memory, in which he described his life between America and Great Britain, was published in 1953. He published his last volume of poems in 1956, A letter to Lucian, and his last book in 1957, The accusing ghost, or justice for Casement.

On 25 June 1958, Alfred Noyes died on the Isle of Wight and was buried in the Roman Catholic cemetery at Freshwater.