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Biodiversity is believed to be closely related to ecosystem functions. However, the ability of existing biodiversity measures, such as species richness and phylogenetic diversity, to predict ecosystem functions remains elusive. Here, we propose a new vector of diversity metrics, structural diversity, which directly incorporates niche space in measuring ecosystem structure. We hypothesize that structural diversity will provide better predictive ability of key ecosystem functions than traditional biodiversity measures. Using the new lidar-derived canopy structural diversity metrics on 19 National Ecological Observation Network forested sites across the USA, we show that structural diversity is a better predictor of key ecosystem functions, such as productivity, energy, and nutrient dynamics than existing biodiversity measures (i.e. species richness and phylogenetic diversity). Similar to existing biodiversity measures, we found that the relationships between structural diversity and ecosystem functions are sensitive to environmental context. Our study indicates that structural diversity may be as good or a better predictor of ecosystem functions than species richness and phylogenetic diversity.