Poor neighborhood conditions are associated with lower levels of physical activity for older adults but socioecological models posit that physical activity depends on both environmental and individual factors. Older adults' ability to overcome environmental barriers to physical activity may partially rely on cognitive resources. However, evidence on the moderating role of these cognitive resources in the associations between environmental barriers and physical activity is still lacking. We analyzed cross-national and longitudinal data on 28,393 adults aged 50 to 96 years as part of the SHARE. Lack of access to services and neighborhood nuisances were used as indicators of poor neighborhood conditions. Delayed recall and verbal fluency were used as indicators of cognitive resources. Confounder-adjusted generalized estimation equations were conducted to test associations between neighborhood conditions and self-reported moderate physical activity, as well as the moderating role of cognitive resources. Results showed that poor neighborhood conditions reduced the odds of engagement in physical activity. Cognitive resources robustly reduced the adverse influence of poor neighborhood conditions on physical activity. Participants with lower cognitive resource scores showed lower odds of engaging in physical activity when neighborhood conditions were poorer, whereas these conditions were not related to this engagement for participants with higher cognitive resource scores. These findings suggest that cognitive resources can temper the detrimental effect of poor neighborhood conditions on physical activity. Public policies should target both individual and environmental factors to tackle the current pandemic of physical inactivity more comprehensively.