This paper examines the association between neighborhood active living potential and walking among middle-aged and older adults. A sample of 2,614 (61.1% women) persons aged 45 years or older and living in one of 112 census tracts in Montreal, Canada, were recruited between February and May of 2005 to participate in a 20-minute telephone survey. Data were linked to observational data on neighborhood active living potential in the 112 census tracts and analyzed through multilevel modeling. Greater density of destinations in the census tract was associated with greater likelihoods of walking for any reason at least 5 days per week for at least 30 minutes (odds ratio = 1.53, 95% confidence interval: 1.21, 1.94). Associations were attenuated but remained statistically significant after controlling for socioeconomic, health, lifestyle, and other physical activity characteristics. Sensitivity analyses showed that associations were robust across smaller and larger volumes of walking. No associations were found between dimensions of neighborhood active living potential and walking for recreational reasons. The authors conclude that a larger number and variety of neighborhood destinations in one's residential environment are associated with more walking and possibly more utilitarian walking among middle-aged or older adults.