Urbanization is associated with higher prevalence of cardiovascular disease worldwide. Aortic stiffness, as measured by carotid-femoral pulse wave velocity is a validated predictor of cardiovascular disease. Our objective was to determine the association between urbanization and carotid-femoral pulse wave velocity. The analysis included 6166 participants enrolled in an ongoing population-based study (mean age 42 years; 58% female) who live in an 80 × 80 km region of southern India. Multiple measures of urbanization were used and compared: 1) census designations, 2) satellite derived land cover (crops, grass, shrubs or trees as rural; built-up areas as urban), and 3) distance categories based on proximity to an urban center. The association between urbanization and carotid-femoral pulse wave velocity was tested in sex-stratified linear regression models. People residing in urban areas had significantly (p < 0.05) elevated mean carotid-femoral pulse wave velocity compared to non-urban populations after adjustment for other risk factors. There was also an inverse association between distance from the urban center and mean carotid-femoral pulse wave velocity: each 10 km increase in distance was associated with a decrease in mean carotid-femoral pulse wave velocity of 0.07 m/s (95% CI: -0.09, -0.06 m/s). The association was stronger among older participants, among smokers, and among those with other cardiovascular risk factors. Further research is needed to determine which components in the urban environment are associated with higher carotid-femoral pulse wave velocity.