Manganese (Mn) is a micronutrient essential for plant growth and a redox-sensitive metal whose bioavailability to microorganisms may play an important role in regulating carbon (C) storage in surface soils (Berg et al., 2015;Jones et al., 2020;Kranabetter, 2019;Stendahl et al., 2017). Bioavailable Mn(II) is released into the solution during litter decomposition and through proton-promoted and reductive dissolution of Mn(III/IV)-oxide minerals that are abundant and ubiquitous in soils (Post, 1999). Plant roots take up soluble Mn(II) from the soil rhizosphere since other existing forms of Mn [Mn(III) and Mn(IV)] are unavailable to plants (Alejandro et al., 2020;Pittman, 2005). Although large reservoirs of Mn(II) can slowly accumulate in woody biomass over a long time-scale, most of the Mn(II) taken up by plants is stored in the foliar tissues each year (Herndon et al., 2015), where Mn concentrations can be up to 12,000 μg g −1 dry-mass (Fernando et al., 2009;Foulds, 1993;St. Clair & Lynch, 2005) with negligible reabsorption during senescence (McCain & Markley, 1989). When Mn returns to soil as Mn(II) in litterfall, it either leaches or is oxidized and converted to Mn(III/IV) oxides as Abstract Manganese (Mn) is an essential plant micronutrient that plays a critical role in the litter decomposition by oxidizing and degrading complex organic molecules. Previous studies report a negative correlation between Mn concentrations and carbon (C) storage in organic horizons and suggest that high Mn concentrations in leaf litter reduce soil C storage in forest ecosystems, presumably by stimulating the oxidation of lignin by fungal enzymes. Yet, the relationship between Mn and C in the litter layer and organic soil remains poorly understood and restricted to a few biomes, hampering our ability to improve mechanistic understanding of soil C accumulation. To examine plant-soil interactions that underlie observed relationships between Mn and C across a wide range of biomes, we extracted biogeochemical data reported for plants and soils from the National Ecological Observatory Network (NEON) database. We found that increased C and nitrogen (N) storage in organic horizons were associated with declines in Mn concentrations across diverse ecosystems at the continental scale, and this relationship was associated with the degree of organic matter decomposition (i.e., O i , O e , and O a ). Carbon and N stocks were more strongly correlated with Mn than with climatic variables (i.e., temperature and precipitation). Foliar Mn was strongly correlated with foliar lignin, and both these parameters increased with a decrease in soil pH, indicating links between soil pH, foliar chemistry, and litter decomposability. Our observations suggest that increased Mn bioavailability and accumulation in foliage under moderately acidic soil conditions support fungal decomposition of lignin-rich litter and contributes to lower soil C stocks.Plain Language Summary Soils contain substantial amounts of carbon that can be stored for hundreds to thousands of ye...