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Vehicle emissions are the most important source of air pollution in the urban environment worldwide, and their detection and control are critical for protecting public health. Here, we report the use of on-road remote sensing (RS) technology for fast, accurate, and cost-effective identification of high-emitting vehicles as an enforcement program for improving urban air quality. Using large emission datasets from chassis dynamometer testing, RS, and air quality monitoring, we found that significant percentages of in-use petrol and LPG vehicles failed the emission standards, particularly the high-mileage fleets. The RS enforcement program greatly cleaned these fleets, in terms of high-emitter percentages, fleet average emissions, roadside and ambient pollutant concentrations, and emission inventory. The challenges of the current enforcement program are conservative setting of cut points, single-lane measurement sites …