Understanding the anthropogenic and natural controls that affect the patterns, distribution, and dynamics of terrestrial carbon is crucial to meeting climate change mitigation objectives. We assessed the human and natural controls over aboveground tree biomass density in African dry tropical forests, using Zambia's first nationwide forest inventory. We identified predictors that best explain the variation in biomass density, contrasted anthropogenic and natural sites at different spatial scales, and compared sites with different stand structure characteristics and species composition. In addition, we evaluated the effects of different management and conservation practices on biomass density. Variation in biomass density was mostly determined by biotic processes, linked with both species richness and dominance (evenness), and to a lesser extent, by land use, environmental controls, and spatial structure. Biomass density was negatively associated with tree species evenness and positively associated with species richness for both natural and human-modified sites. Human influence variables (including distance to roads, distance to town, fire occurrence, and the population on site) did not explain substantial variation in biomass density in comparison to biodiversity variables. The relationship of human activities to biomass density in managed sites appears to be mediated by effects on species diversity and stand structure characteristics, with lower values in human-modified sites for all metrics tested. Small contrasts in carbon density between human-modified and natural forest sites signal the potential to maintain carbon in the landscape inside but also outside forestlands in this region. Biodiversity is positively related to biomass density in both human and natural sites, demonstrating potential synergies between biodiversity conservation and climate change mitigation. This is the first evidence of positive outcomes of protected areas and participatory forest management on carbon storage at national scale in Zambia. This research shows that understanding controls over biomass density can provide policy relevant inputs for carbon management and on ecological processes affecting carbon storage.