Background: Few studies have assessed built environment correlates of active commuting in low-and-middle-income countries, but the different context could yield distinct findings. This cross-sectional study investigated associations between home neighbourhood environment characteristics and active commuting in Chennai, India. Methods: Adults (N = 370, 47.2% female, mean age = 37.9 years) were recruited from 155 wards in the metropolitan area of Chennai in southern India between January and June 2015. Participants self-reported their usual mode of commute to work, with responses recoded into three categories: (1) multi-modal or active commuting (walking and bicycling); (2) public transit; and (3) private transport. Environmental attributes around participants’ homes were assessed using the Neighborhood Environment Walkability Scale-India (NEWS-India). Associations between environmental characteristics and likelihood of active commuting and public transit use were modelled using logistic regression with private transport (driving alone or carpool) as the reference category, adjusting for age, gender, and household car ownership. Results: Consistent with other international studies, participants living in neighbourhoods with a mix of land-uses and a transit stop within a 10-minute walk from home were more likely to use active commuting (both p < 0.01). Land-use mix was significantly associated with the use of public transit compared to private transport (aOR = 5.2, p = 0.002). Contrary to findings in high-income countries, the odds of active commuting were reduced with improved safety from crime (aOR = 0.2, p = 0.003), aesthetics (aOR = 0.2, p = 0.05) and street connectivity (aOR = 0.2, p = 0.003). Conclusions: Different environmental attributes were associated with active commuting, suggesting that these relationships are complex and may distinctly differ from those in high-income countries. Unexpected inverse associations of perceived safety from crime and aesthetics with active commuting emphasize the need for high quality epidemiologic studies with greater context-specificity in the study of physical activity in LMICs. Findings have public health implications for India and suggest that caution should be taken when translating evidence across countries.