Significance: Green spaces have a range of health benefits, but little is known in relation to cognitive development in children. This study, based on comprehensive characterization of outdoor surrounding greenness (at home, school, and during commuting) and repeated computerized cognitive tests in schoolchildren, found an improvement in cognitive development associated with surrounding greenness, particularly with greenness at schools. This association was partly mediated by reductions in air pollution. Our findings provide policymakers with evidence for feasible and achievable targeted interventions such as improving green spaces at schools to attain improvements in mental capital at population level.