Significance Previous estimations of carbon budgets in China’s terrestrial ecosystems varied greatly because of the multiplicity of data sources and the inconsistency of methodologies. By conducting a methodologically consistent field campaign across the country, we estimated that the total carbon pool in China’s forests, shrublands, grasslands, and croplands was 79.24 ± 2.42 Pg C. The carbon density exhibited a strong dependence on climate regime: it decreased with temperature but increased with precipitation. The country’s forests have a large potential of biomass carbon sequestration of 1.9–3.4 Pg C in the next 10 to 20 years assuming no removals. Our findings provide a benchmark to identify the effectiveness of the government’s natural protection policies.