Le Grice started his career as a painter but began to make film and computer works in the mid 1960s,[5] becoming a pioneer of computer-generated filmmaking.

[9] His work was screened at the Museum of Modern Art, the Louvre and the Tate Modern and Tate Britain and is in permanent collections including: the Centre Pompidou, the Cinematek, the National Film and Sound Archive, Deutsche Kinemathek, Canadian Distribution Centre, Montreal and Archives du Film Experimental D'Avignon.

A number of his longer films were transmitted on British television, including Finnegans Chin, Sketches for a Sensual Philosophy and Chronos Fragmented.

Le Grice wrote critical and theoretical works including a history of experimental cinema, titled Abstract Film and Beyond (1977, Studio Vista and MIT).

For three years in the 1970s he wrote a regular column for the art monthly Studio International and published numerous other articles on film, video and digital media.