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Abstract China has large, estimated potential for direct air carbon capture and storage (DACCS) but its deployment locations and impacts at the subnational scale remain unclear. This is largely because higher spatial resolution studies on carbon dioxide removal (CDR) in China have focused mainly on bioenergy with carbon capture and storage. This study uses a spatially detailed integrated energy-economy-climate model to evaluate DACCS for 31 provinces in China as the country pursues its goal of climate neutrality by 2060. We find that DACCS could expand China’s negative emissions capacity, particularly under sustainability-minded limits on bioenergy supply that are informed by bottom-up studies. But providing low-carbon electricity for multiple GtCO₂yr⁻¹DACCS may require over 600 GW of additional wind and solar capacity nationwide and comprise up to 30% of electricity demand in China’s northern provinces. Investment requirements for DACCS range from $330 to $530 billion by 2060 but could be repaid manyfold in the form of avoided mitigation costs, which DACCS deployment could reduce by up to $6 trillion over the same period. Enhanced efforts to lower residual CO₂emissions that must be offset with CDR under a net-zero paradigm reduce but do not eliminate the use of DACCS for mitigation. For decision-makers and the energy-economy models guiding them, our results highlight the value of expanding beyond the current reliance on biomass for negative emissions in China.