BACKGROUND:  The neighborhood environment may play a role in encouraging sedentary patterns, especially for middle-aged and older adults.  PURPOSE:  The aim of this study was to examine the associations between walking and neighborhood population density, retail availability, and land-use distribution using data from a cohort of adults aged 45 to 84 years.  METHODS:  Data from a multi-ethnic sample of 5529 adult residents of Baltimore MD, Chicago IL, Forsyth County NC, Los Angeles CA, New York NY, and St. Paul MN enrolled in the Multi-Ethnic Study of Atherosclerosis in 2000–2002 were linked to secondary land-use and population data. Participant reports of access to destinations and stores and objective measures of the percentage of land area in parcels devoted to retail land uses, the population divided by land area in parcels, and the mixture of uses for areas within 200 m of each participant's residence were examined. Multinomial logistic regression was used to investigate associations of self-reported and objective neighborhood characteristics with walking. All analyses were conducted in 2008 and 2009.  RESULTS:  After adjustment for individual-level characteristics and neighborhood connectivity, it was found that higher density, greater land area devoted to retail uses, and self-reported proximity of destinations and ease of walking to places were each related to walking. In models including all land-use measures, population density was positively associated with walking to places and with walking for exercise for more than 90 minutes/week, both relative to no walking. Availability of retail was associated with walking to places relative to not walking, and having a more proportional mix of land uses was associated with walking for exercise for more than 90 minutes/week, while self-reported ease of access to places was related to higher levels of exercise walking, both relative to not walking.  CONCLUSIONS:  Residential density and the presence of retail uses are related to various walking behaviors. Efforts to increase walking may benefit from attention to the intensity and type of land development.