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The art collection housed in the Picture Gallery at Royal Holloway College was based on the similar model at Vassar College in America. Thomas Holloway compiled the collection through purchases at auction from 1881-1883, when he bought at every Christie's sale of note. Although the initial plan was to obtain modern British paintings, examples of work by European painters were also acquired. The collection totalled 77 pictures at the time of Holloway's death in 1883. Charles W Carey was appointed to act as Curator of the Picture Gallery, a task he undertook from 1887 until his death in 1943.
His main role was to supervise the conservation of the pictures, compile the catalogue, show the collection to visitors, and correspond with artists, art historians and students concerning the works.