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Abstract Decomposition is the transformation of dead organic matter into its inorganic constituents. In most biomes, decomposition rates can be accurately predicted with simple mathematical models, but these models have long under‐predicted decomposition in globally extensive drylands.We posit that the exposed surface conditions characteristic of drylands make litter decomposition uniquely subject to microsite‐specific environmental controls and spatially variable microbial communities. As such, decomposition in dryland ecosystems—which are characterized by extremes in temporal heterogeneity of climate conditions and spatial heterogeneity of vegetation cover with corresponding microclimate variability—is a prime example of a macrosystems process that can be addressed by merging field data with new predictive process models operating across a hierarchical continuum of spatial scales and process resolutions.A macrosystems approach offers promise to reconcile model‐measurement discrepancies by integrating observations and experiments across multiple scales, from microsites (e.g. shrub sub‐canopy or intercanopy) to regions (e.g. across a 100s of km²study site with complex topography, precipitation and temperature) and ultimately to a continental perspective (e.g. North American drylands).Recent developments in technology and data availability position the scientific community to integrate laboratory, field, modelling and remote sensing approaches across a hierarchical range of scales to capture the spatiotemporal distribution of litter and environmental conditions needed to predict decay dynamics at the micro‐to‐macroscale. This multi‐scale approach promises a path forward to resolving a longstanding disconnect between measured data and modelled processes in dryland litter decomposition.Dryland litter decomposition presents an excellent case study for resolving spatially and temporally complex biogeochemical dynamics through a hierarchical, multidisciplinary macrosystems approach.We focus on dryland litter decomposition, but the hierarchical, multidisciplinary macrosystems approach we outline shows great potential for resolving other spatially and temporally complex biogeochemical processes across a wide range of ecosystems. Read the freePlain Language Summaryfor this article on the Journal blog.