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Whether crime or the perception of it has any direct and significant influence on travelers’ mode choice is a topic for which the evidence remains inconclusive. Studies have revealed various, and in some cases counterintuitive, roles that safety concerns can play in individuals’ travel behavior. In addition, characteristics of the physical environment such as land use and walkability are also influential factors in travelers’ decisions. This study explored these questions through the study of individual travel behavior by using discrete choice models applied to the reported home-based work trips in the Chicago household travel survey. Mode choice was modeled as functions of variables such as sociodemographics, neighborhood crime density (as a safety measure), and walk score (as a measure of walkability). Different crime types were examined, and a crime index was introduced. Results suggest that both walk score and the crime index at the destination can be considered meaningful predictors of individuals’ mode usage. The crime index at origin, however, does not show a significant and meaningful effect.