Resource-based cities generally have large carbon-emission, and their carbon balance status is receiving more attention. Land use is a key factor in regulating regional carbon balance. To explore the relationship between land use patterns and carbon balance in resource-based cities, we selected nine cities in Anhui, a major energy province, as the research object. Based on the land use data (2000–2020) and the carbon emission coefficient method, we calculated the carbon emissions, carbon sequestration, and net carbon emissions to show their spatiotemporal evolution. The Logarithmic Mean Divisia Index (LMDI) method was employed to explore the driving factors of carbon emissions. The results indicated the following: (1) Net carbon emissions increased by 149.60%, and the growth rate had slowed down since 2015. Forestland constituted the primary carbon sink, whereas cropland was the dominant carbon source. The spatial distribution of carbon emissions and carbon sequestration was uneven. (2) The economic development level and energy consumption density were the principal factors of emission increases. Conversely, carbon emission intensity and land use economic efficiency served as the key mitigating factors.