Land use and land cover change mainly affect the carbon cycle process in the terrestrial ecosystem. In the context of achieving carbon neutrality, it is of practical significance to analyze regional carbon balance and optimize land use structure. Taking 1 km grid as the unit and Henan Province as an example, this paper used InVEST carbon sequestration module, IPCC carbon emission accounting method, and population density method to study the spatio-temporal changes of regional carbon balance in 1995, 2005, and 2015. The results show that the supply and demand of carbon sequestration services in the study area are closely related to land use types. There is a spatial mismatch between supply and demand of carbon sequestration services, that is, areas with high demand usually have low supply. During the study period, the total carbon sequestration in the study area decreased year by year, while the total carbon emissions increased year by year. The carbon balance in the study area showed an overall positive trend, while local deterioration. Based on the analysis of carbon balance, some suggestions on spatial optimization are put forward, which can provide reference for the realization of carbon balance target of national spatial planning in the future.