This work focuses on the concentration and health effects of volatile organic compounds (VOCs) at an intercity bus terminal in Taipei City, Taiwan. In this study, 36 VOCs were detected in the bus terminal, including 19 hazardous air pollutants. The measurement results indicate that ethanol, acetone, toluene, and methyl tert-butyl ether (MTBE) were the main VOCs dominating this bus terminal. Moreover, the average concentration of benzene, toluene, ethylbenzene, and xylene (BTEX) compounds was 106.0 μg/m³ inside the bus terminal, contributing to approximately 70% of the hazardous air pollutants. The measurement results suggest that traffic emissions, especially from diesel buses, were the major pollution sources in the bus terminal. The cancer risk for 1,3-butadiene, benzene, ethylbenzene, and naphthalene exceeded the suggested value by the U.S. EPA. In addition, the individual chronic hazard quotient of benzene was higher than the recommended level. The findings of this work imply that bus terminal workers face a potential health risk, which is a matter of concern.