Lyttle was an early collector and producer of LSD blotter art. He is the person who first conceived of asking psychedelic celebrities like Albert Hofmann, Timothy Leary, Sasha Shulgin, Annie Sprinkle, Peter Fonda, Alex Grey, Laurence Gartel, HR Giger, and others to autograph undipped sheets of blotter. This action inspired increased interest of blotter as an art form. Signed blotter became highly collectible, with rare sheets selling for hundreds or thousands of dollars. Before his death, Lyttle donated some of his more valuable pieces of blotter art to the Multidisciplinary Association for Psychedelic Studies, and the sale of autographed blotter raised around $20,000 for MAPS.