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There is growing interest in identifying neighborhood environment factors related to physical activity.This study aimed to examine whether objective built (e.g., residential density) and perceived (e.g., aesthetics) environment factors around adults’ residence are correlates of their physical activity and reported walking behavior after accounting for known psychosocial (e.g., self-efficacy, barriers to physical activity) and demographic correlates of physical activity.Objective built environment characteristics were created through network buffers around individual participants (n = 2199) selected from neighborhoods differing on walkability characteristics and household income. Participants wore accelerometers to obtain a more objective measure of overall physical activity and self-reported on leisure and transportation-related walking, perceptions of neighborhood environment, psychosocial factors related to physical activity, and demographic factors. Census-level demographic factors were also considered.Retail floor area ratio, a metric combining land use mix and pedestrian design factors, was the environmental factor most related to accelerometry-measured physical activity and self-reported transportation-related walking after accounting for psychosocial and demographic factors. Street connectivity was also related to transportation-related walking, whereas perceived aesthetics was positively related to leisure walking.Environmental factors, particularly the availability of proximal nonresidential destinations designed for pedestrian access, were related to adults’ physical activity and walking after accounting for psychosocial and demographic correlates, including reasons for residential selection.