This study develops a bottom-up model to quantitatively assess the comprehensive effects of replacing traditional petroleum-powered vehicles with natural gas vehicles (NGVs) in China based on an investigation of the direct energy consumption and critical air pollutant (CAP) emission intensity, life-cycle energy use and greenhouse gas (GHG) emission intensity of NGV fleets. The results indicate that, on average, there are no net energy savings from replacing a traditional fuel vehicle with an NGV. Interestingly, an NGV results in significant reductions in direct CAP and life-cycle GHG emissions compared to those of a traditional fuel vehicle, ranging from 61% to 76% and 12% to 29%, respectively. Due to the increasing use of natural gas as a vehicle fuel in China (i.e. approximately 28.2 billion cubic metres of natural gas in 2015), the total petroleum substituted with natural gas was approximately 23.8 million tonnes (Mt), which generated a GHG emission reduction of 16.9 Mt of CO 2 equivalent and a CAP emission reduction of 1.8 Mt in 2015. Given the significant contribution of NGVs, growing the NGV population in 2020 will further increase the petroleum substitution benefits and CAP and GHG emission reduction benefits by approximately 42.5 Mt of petroleum-based fuel, 3.1 Mt of CAPs and 28.0 Mt of GHGs. By 2030, these benefits will reach 81.5 Mt of traditional petroleum fuel, 5.6 Mt of CAPs and 50.5 Mt of GHGs, respectively.