The collection primarily consists of 189 letters addressed to Sir Thomas Henry Hall Caine, a prominent British novelist and secretary to Dante Gabriel Rossetti, the poet and painter. The bulk of the correspondence is hand-written signed letters. There are many typed signed letters, along with other forms of correspondence, such as a telegram. Caine lived from May 14, 1853 until August 31, 1931. Caine greatly admired Rosetti and the Pre-Raphaelite writings and much of the correspondence centers around the movement. Literary themes, especially related to events of the day, predominate the subjects of the letters. Many prominent intellectuals wrote to Caine, including Sir James M. Barrie, the author of Peter Pan; Sir Arthur Wing Pinero, a leading playwright of the late Victorian and Edwardian periods; Archibald Philip Primrose, 5th Earl of Rosebery and British prime minister from 1894 to 1895; Israel Zangwill, a writer and Zionist; Sir Arthur Conan Doyle, a Scottish writer best known for his series of stories about Sherlock Holmes; and Sir Walter Besant, an English novelist and philantropist.

Correspondence in this collection is contained within one letter-sized document case measuring .5 cubic feet. The collection is arranged alphabetically by the writer's name and chronologically if there is more than one letter by the writer. The only exceptions to this arrangement are the personal files of Caine containing personal papers and family correspondence. The collection is in good condition.