Transportation-related physical activity can significantly increase daily total physical activity through active transportation or walking/biking to transit stops. The purpose of this study was to assess the relations between transit-use and self-reported and monitor-based physical activity levels in a predominantly minority population from the Houston Travel-Related Activity in Neighborhoods (TRAIN) Study. This was a cross-sectional analysis of 865 adults living in Houston, Texas between 2013 and 2015. The exposure variable was transit-use (non-users, occasional users, and primary users). Self-reported and accelerometer-determined physical activity were the outcomes of interest. Regression models adjusting for age, sex, race/ethnicity, and other covariates of interest were built to test the hypothesis that transit user status was directly associated with 1) minutes of moderate-intensity physical activity and 2) the prevalence of achieving the physical activity guidelines. The majority of participants were female, non-Hispanic black, and almost one-third had a high school education or less. After adjustment, primary transit-use was associated with 134.2 (p < 0.01) additional mean minutes per week of self-reported moderate-intensity transportation-related physical activity compared to non-users. Further, primary users had 7.3 (95% CI: 2.6–20.1) times the relative adjusted odds of meeting physical activity recommendations than non-users based on self-reported transportation-related physical activity. There were no statistically significant associations of transit-use with self-reported leisure-time or accelerometer-derived physical activity. Transit-use has the potential for a large public health impact due to its sustainability and scalability. Therefore, encouraging the use of transit as a means to promote physical activity should be examined in future studies.