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Charles William Jefferys was born in Rochester, England in 1869. In 1877, he emigrated with his family to Philadephia, eventually moving to Toronto in 1881. With little formal schooling, he was apprenticed from 1885 to 1890 at the Toronto Lithography Company. He joined the Toronto Art Students' League in 1888 and studied watercolour painting under Charles MacDonald Manly. Jefferys worked as a news illustrator for The Toronto Globe from 1889 to 1892 before moving to New York, where he worked at The New York Herald.
Jefferys returned to Toronto in 1901, where he had a long career as a newspaper, magazine, and book illustrator, creating the illustrations for titles including The Chronicles of America, Episodes in Canada's Story, Canada's Past in Pictures, and the three-volume Picture Gallery of Canadian History. He also taught painting and drawing in the Department of Architecture at the University of Toronto from 1912 to 1929. Later work included guiding the reconstruction of the Habitation at Port-Royal, Nova Scotia in 1938 and painting the murals at the Royal Ontario Museum. Jefferys was a founder of the Canadian Authors' Association, a councillor of the Royal Academy of Arts, and served as president for the Ontario Society of Artists and the Canadian Society of Graphic Arts.
In 1915, Jefferys drew over one hundred sketches to illustrate a projected series on the works of Thomas Chandler Halliburton. The project never came to fruition and the illustrations were published posthumously in the 1956 volume Sam Slick in Pictures.
Jefferys passed away in 1951.