The gallery's collection originally was focused on artists of local residence and art of local subject matter. The earliest exhibits were of watercolourist George Chauvignaud, a painter from Peel in the 1920s and 1930s, as well as a show of Brampton-born printmaker Caroline Armington, based on a donation by Caroline Crawford.
In more recent decades, the collection has expanded to include several hundred works, from throughout the development of 20th century abstraction in Canada. The selection includes works by early movements, such as Les Automatistes and Painters Eleven, and contemporary figures in non-objective painting, such as David Urban and Ric Evans. Other artists noted in gallery materials include Harold Town, Jack Bush, Claude Tousignant, Guido Molinari, Ron Martin, Chris Cran, William Ronald, John Meredith, and Ronald Bloore; the final three in the list were once Brampton residents.
The collection includes various major works by national-level artists, designated with the Canadian Cultural Property status.
Artists mentioned in publicity for the gallery include John Anderson, Caroline Armington, Frank Armington, John Armstrong, Carl Beam, George Broomfield, Alex Cameron, Chuck Close, Tom Dean, Mary Dignam, Leonard J. Hutchinson, Tom LaPierre, Doris McCarthy, David Milne, Robert Motherwell, Will Ogilvie, Stephanie Rayner, Jim Reid, Jack Shadbolt, Michael Snow, Stanley Spencer, Tom Stone, Andy Warhol, and Joyce Weiland. A Tom Thomson sketchbook is included in the collection.
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