Background:India is undergoing rapid urbanization with simultaneous increases in the prevalence of cardiovascular disease (CVD). As urban areas become home to an increasing share of the world’s population, it is important to understand relationships between the built environment and progression towards CVD.Objective:We assessed associations between multiple measures of the built environment and biomarkers of early vascular aging (EVA) in the Population Study of Urban, Rural and Semiurban Regions for the Detection of Endovascular Disease and Prevalence of Risk Factors and Holistic Intervention Study (PURSE-HIS) in Chennai, India.Methods:We performed a cross-sectional analysis of 3,150 study participants. EVA biomarkers included systolic and diastolic blood pressure (SBP and DBP), central pulse pressure (cPP) and flow-mediated dilatation (FMD). Multiple approaches were used to assign residential exposure to factors of the built environment: Moderate Resolution Imaging Spectroradiometer (MODIS)-derived normalized difference vegetation index (NDVI), a measure of vegetation health and greenness; Landsat-derived impervious surface area (ISA); and Visible Infrared Imaging Radiometer Suite (VIIRS)-derived nighttime lights (NTL). Multivariable regression models were used to assess associations between each built environment measure and biomarkers of EVA, adjusting for age, body mass index (BMI), cooking fuel type, energy intake, sex, physical activity, smoking, socioeconomic status, and stress.Results:Residing in areas with higher ISA or NTL, or lower greenness, was significantly associated with elevated SBP, DBP, and cPP, and with lower FMD, adjusting for age, BMI, sex, smoking status, and other CVD risk factors. An interquartile range decrease in greenness had the largest increase in SBP [4.3 mmHg (95% CI: 2.9, 5.6)], DBP [1.2 mmHg (95% CI: 0.4, 2.0)] and cPP [3.1 mmHg (95% CI: 2.0, 4.1)], and the largest decrease in FMD [−1.5% (95%CI: −2.2%, −0.9%].Conclusion:Greenness, ISA, and NTL were associated with increased SBP, DBP, and cPP, and with reduced FMD, suggesting a possible additional EVA pathway for the relationship between urbanization and increased CVD prevalence in urban India. https://doi.org/10.1289/EHP541