A case study approach is used to present causal evidence from the United Kingdom on the impact of neighborhood design on travel behavior. “Sustainable travel to work” is defined as including walking, cycling, and travel by bus or light rail. Travel-to-work data are derived from the British Census 2001 for two groups of carefully selected neighborhoods–- those exhibiting either a high or a low incidence of sustainable travel-to-work patterns. A questionnaire was used to capture dimensions of neighborhood attitudes and preferences, socioeconomic characteristics, and car-travel characteristics in the northeast of England. The results offer microscale evidence by using a cross-sectional design to investigate the relationship between neighborhood characteristics and travel behavior and by using multivariate analysis to explore differences between neighborhood groups for socioeconomic variables, travel attitudes, and perceived neighborhood characteristics. The neighborhood group with a high incidence of sustainable travel to work is shown to have a higher potential to travel farther, and the neighborhood group with a low incidence of sustainable travel to work is shown to have a higher potential to use public transport. These results imply a policy dilemma about how public preferences for improved travel accessibility should be met by local authorities.