Understanding the relationship between biodiversity and productivity can be advanced by improving metrics used to quantify biodiversity. Structural diversity, that is, variation of size and form of plant organs, is an emerging biodiversity metric. However, compared with the other biodiversity metrics, its relative importance in specific components of forest productivity, for example, recruitment of new individuals, biomass net change after accounting for mortality, is largely unknown, particularly across a large spatial scale with multiple influential gradients. To address the knowledge gap, we used USDA Forest Service Forest Inventory and Analysis (FIA) data across the southcentral USA from 2008 to 2017. We calculated forest biomass increments due to recruitment and growth and net change in biomass. Then, we quantified the effects of a range of abiotic and biotic variables on the biomass increments and net change. Our results showed that (1) Structural diversity was negatively associated with the two biomass increments and net change in biomass. The negative effects were supported by increased occurrences of insects and diseases with greater structural diversity. (2) Compared with species and functional diversity, structural diversity showed a better association with biomass increments and net change, suggested by its larger absolute values of standardized coefficients, and the effects of structural diversity were negative in contrast to species diversity. (3) The effects of structural diversity, stand age, and elevation differed between natural and planted forests that may stem from the differences in stand development and species composition between the two forest types. Together, structural diversity may represent an important dimension of biodiversity impacts on plant productivity, which could be related to the exacerbated disturbances with greater structural diversity.