Objective: To investigate the associations between perceived environment features and walking in older adults. Method: A cross-sectional population-based study was performed in Florianopolis, Brazil, including 1,705 older adults (60+ years). Walking was measured by the International Physical Activity Questionnaire (IPAQ), and perceived environment was assessed through the Neighborhood Environment Walkability Scale. We conducted a multinomial logistic regression to examine the association between perceived environment and walking. Results: The presence of sidewalks was related to both walking for transportation and for leisure. Existence of crosswalks in the neighborhood, safety during the day, presence of street lighting, recreational facilities, and having dog were significant predictors of walking for transportation. Safety during the day and social support were significantly associated with walking for leisure. Discussion: The perceived environment may affect walking for specific purposes among older adults. Investments in the environment may increase physical activity levels of older adults in Brazil.