Living in neighborhoods with lower incomes, lower education/occupational levels, and/or higher crime increases one’s risk of developing chronic health problems including cardiovascular disease risk factors and stroke. These cardiovascular health problems are known to contribute to cognitive decline and dementia. The purpose of this study was to determine the association of neighborhood socioeconomic resources and crime-related psychosocial hazards on stroke risk and cognition, hypothesizing that cardiovascular health would mediate any relationship between the neighborhood-level environment and cognition. The study evaluated 121 non-demented Chicago-area adults (~67 years; 40% non-Latino White) for cardiovascular health problems using the Framingham Stroke Risk Profile 10-year risk of stroke (FSRP-10). The cognitive domains that were tested included memory, executive functioning, and attention/information processing. Neighborhood socioeconomic resources were quantified at the census tract level (income, education, and occupation); crime-related psychosocial hazards were quantified at the point level. Structural equation modeling (SEM) did not show that the FSRP-10 mediated the relationship between neighborhood characteristics and domain-specific cognition. The SEM results did suggest that higher crime rates were associated with a higher FSRP-10 (β(105) = 2.38, p = 0.03) and that higher FSRP-10 is associated with reduced attention/information processing performance (β(105) = −0.04, p = 0.02) after accounting for neighborhood socioeconomic resources. Clinicians may wish to query not only individual but also neighborhood-level health when considering cognition.