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Recent studies report that multifunctionality-the simultaneous provision of multiple ecosystem functions-in drylands depends on biodiversity. Others report that specific size distributions of vegetation patches indicate overall ecosystem health and function. Using a biocrust (micro-vegetation of mosses, lichens, and cyanobacteria) model system, and multivariate modeling, we determined the relative importance of biodiversity, patch-size distribution, and total abundance to nutrient cycling and multifunctionality. In most cases we explained at least 20%, and up to 65%, of the variation in ecosystem functions, and 42% of the variation in multifunctionality. Species richness was the most important determinant of C cycling, constituting an uncommonly clear link between diversity and function in a non-experimental field setting. Regarding C cycling in gypsiferous soils, we found that patch size distributions with a greater frequency of small to medium patches, as opposed to very small patches, were more highly functional. Nitrogen cycling was largely a function of biocrust cover in two soil types, whereas in gypsiferous soils, more central-tending patch size distributions were less functional with regards to N cycling. All three community properties were about equally important to multifunctionality. Our results highlight the functional role of biotic attributes other than biodiversity, and indicate that high cover and diversity, together with a particular patch-size distribution, must be attained simultaneously to maximize multifunctionality. The results also agree with trends observed with other terrestrial and aquatic communities that more biodiversity is needed to sustain multifunctionality compared to single functions considered independently.