Born in London, Walker took an active role in many organisations that were at the heart of the Arts and Crafts movement, including the Art Workers Guild, the Society for the Protection of Ancient Buildings and the Arts and Crafts Exhibition Society.
In the late 1870s Walker frequented William Morris, with whom he shared both Socialist beliefs and a keen interest in printing. Walker's collection of 16th-century typefaces inspired Morris to create the Kelmscott Press. After Morris' death, Walker set up his own printing enterprise, the Doves Press, with bookbinder T. J. Cobden Sanderson which in turn inspired the private presses of the 20th century.
In 1910, he photographed the Rice portrait of Jane Austen, subsequently published in the 1913 edition of Jane Austen: her life and letters, a family record by William Austen-Leigh and Richard Arthur Austen-Leigh.
Walker's daughter, Dorothy Walker, and later Dorothy's live-in companion, Elizabeth de Haas, preserved many of Walker's private papers and the family collection of Arts and Crafts decorative items and ephemera at the family home at 7, Hammersmith Terrace, London. The house is now a museum run by the Emery Walker Trust.
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