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• Source reduction contributes greatly to VOC emission reduction. • A comprehensive assessment system helps tailor effective VOC control strategies. • A comprehensive assessment system helps to improve reduction targeting. • Synergistic control of the overall process promotes VOC reduction benefits. Strong volatile organic compound (VOCs) emissions from solvent-using industries are one of the most pressing environmental challenges in China, and urgently require a cost-effective and carbon-reduction benefit synergistic control strategy. Here, we proposed a novel comprehensive assessment system to optimize a whole-process control strategy that can simultaneously meet triple goals of reduction potential, cost-benefits, and carbon reduction. By focusing on Inner Mongolia Autonomous Region, Shenzhen City, Lanzhou City, Nanyang City and Shunde District of Foshan City, each exhibiting different emission characteristics in packaging and printing (P&P) industry, we proposed various synergistic control strategies and options for reduction potential, cost-benefits, and carbon reduction. This new comprehensive assessment system was shown to be beneficial for obtaining a coordinated control option with better comprehensive effects. Overall our results indicate how to formulate efficient policies, optimized for different regions, to mitigate VOC pollution in industrial sectors. [Display omitted] [ABSTRACT FROM AUTHOR]