Decomposition models typically under-predict decomposition relative to observed rates in drylands. This discrepancy indicates a significant gap in our mechanistic understanding of carbon and nutrient cycling in these systems. Recent research suggests that certain drivers of decomposition that are often not explicitly incorporated into models (e.g., photodegradation and soil-litter mixing; SLM) may be important in drylands, and their exclusion may, in part, be responsible for model under-predictions. To assess the role of SLM, litterbags were deployed in the Chihuahuan Desert and interrelationships between vegetation structure, SLM, and rates of decomposition were quantified. Vegetation structure was manipulated to simulate losses of grass cover from livestock grazing and shrub encroachment.We hypothesized that (i) reductions in grass cover would destabilize soils and promote SLM, and (ii) that SLM would enhance microbial abundance and alter microbial community composition in ways that accelerate decomposition. To test our hypotheses, we quantified mass loss, and chemistry of litter incubated on sites with experimental reductions in grass cover (0 to 100% removals) over a 12-month period. This dataset includes data pertaining to the percent carbon, percent nitrogen, and the carbon to nitrogen ratio. This study is complete.