Physical inactivity among children is on the rise. Active transport to school (ATS), namely walking and cycling there, adds to children's activity level. Little is known about how exposures along actual routes influence children's transport behavior. This study examined how natural and built environments influence mode choice among Dutch children aged 6–11 years. 623 school trips were tracked with global positioning system. Natural and built environmental exposures were determined by means of a geographic information system and their associations with children's active/passive mode choice were analyzed using mixed models. The actual commuted distance is inversely associated with ATS when only personal, traffic safety, and weather features are considered. When the model is adjusted for urban environments, the results are reversed and distance is no longer significant, whereas well-connected streets and cycling lanes are positively associated with ATS. Neither green space nor weather is significant. As distance is not apparent as a constraining travel determinant when moving through urban landscapes, planning authorities should support children's ATS by providing well-designed cities.