The Climate Change Conference of Parties (COP) 21 in December 2015 established Nationally Determined Contributions toward reduction of greenhouse gas emissions. In the years since COP21, it has become increasingly evident that carbon dioxide removal (CDR) technologies must be deployed immediately to stabilize concentration of atmospheric greenhouse gases and avoid major climate change impacts. Biochar is a carbon-rich material formed by high-temperature conversion of biomass under reduced oxygen conditions, and its production is one of few established CDR methods that can be deployed at a scale large enough to counteract effects of climate change within the next decade. Here we provide a generalized framework for quantifying the potential contribution biochar can make toward achieving national carbon emissions reduction goals, assuming use of only sustainably supplied biomass, i.e., residues from existing agricultural, livestock, forestry and wastewater treatment operations. Our results illustrate the significant role biochar can play in world-wide CDR strategies, with carbon dioxide removal potential of 6.23 ± 0.24% of total GHG emissions in the 155 countries covered based on 2020 data over a 100-year timeframe, and more than 10% of national emissions in 28 countries. Concentrated regions of high biochar carbon dioxide removal potential relative to national emissions were identified in South America, northwestern Africa and eastern Europe. Graphical abstract