Few longitudinal residential relocation studies have explored associations between urban form and physical activity, and none has used the Space Syntax theory. Using a Canadian longitudinal dataset (n = 5944), we estimated: (1) differences in physical activity between non-movers, and those relocating to neighbourhoods with less or more integrated street layouts, and; (2) associations between changes in street layout integration exposure and differences in physical activity. Adjusting for covariates, we found relative to non-movers, those who moved to more integrated neighbourhoods undertook significantly (p < .05) more leisure walking (27.3 min/week), moderate-intensity (45.7 min/week), and moderate-to-vigorous intensity physical activity (54.4 min/week). Among movers, a one-unit increase in the relative change in street integration exposure ([Street integration at follow-up-street integration at baseline]/street integration at baseline) was associated with a 7.5 min/week increase in leisure walking. Our findings suggest that urban design policies that improve neighbourhood street integration might encourage more physical activity in adults.