Increasing soil carbon storage is an important strategy for achieving sustainable development. Enhancing soil carbon sequestration capacity can effectively reduce the concentration of atmospheric carbon dioxide, which not only contributes to the carbon neutrality goal but also helps maintain ecosystem stability. Based on 146 soil samples collected at plot locations selected across Beijing, we examined relationships between soil organic carbon (SOC) and key characteristics of urban forests, including their spatial structure and species complexity. The results showed that SOC in the topsoil with a depth of 20 cm was highest over forested plots (6.384 g/kg–20.349 g/kg) and lowest in soils without any vegetation cover (5.586 g/kg–6.783 g/kg). The plots with herbaceous/shrub vegetation but no tree cover had SOC values in between (5.586 g/kg–15.162 g/kg). The plot data revealed that SOC was better correlated with the physical structure than the species diversity of Beijing’s urban trees. The correlation coefficients (r) between SOC and five physical structure indicators, including average diameter at breast height (DBH), average tree height, basal area density, and the diversity of DBH and tree height, ranged from 0.32 to 0.52, whereas the r values for four species diversity indicators ranged from 0.10 to 0.25, two of which were not statistically different from 0. Stepwise linear regression analyses revealed that the species diversity indicators were not very sensitive to SOC variations among a large portion of the plots and were about half as effective as the physical structure indicators for explaining the total variance of SOC. These results suggest that urban planning and greenspace management policies could be tailored to maximize the carbon co-benefits of urban land. Specifically, trees should be planted in urban areas wherever possible, preferably as densely as what can be allowed given other urban planning considerations. Protection of large, old trees should be encouraged, as these trees will continue to sequester and store large quantities of carbon in above- and belowground biomass as well as in soil. Such policies will enhance the contribution of urban land, especially urban forests and other greenspaces, to nature-based solutions (NBS) to climate change.