SignificanceDeploying coal-bioenergy gasification systems with carbon capture and storage (CBECCS) provides a promising opportunity for China to realize its carbon mitigation and air pollution abatement goals simultaneously. We conducted a comprehensive assessment of CBECCS technology for China, with a focus on plant and fuel configurations (e.g., biomass ratios) and economics, as well as CO₂and greenhouse gas emissions and cobenefits for air quality. We find significant opportunities for carbon mitigation with air quality cobenefits from deployment of CBECCS systems in regions that are both rich in crop residues and facing urgent needs to curb serious air pollution. The study thus provides critical information for policy makers seeking to exploit the carbon-negative energy opportunities of CBECCS technology.