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Abstract Identifying controls on soil organic carbon (SOC) storage, and where SOC is most vulnerable to loss, are essential to managing soils for both climate change mitigation and global food security. However, we currently lack a comprehensive understanding of the global drivers of SOC storage, especially with regards to particulate (POC) and mineral‐associated organic carbon (MAOC). To better understand hierarchical controls on POC and MAOC, we applied path analyses to SOC fractions, climate (i.e., mean annual temperature [MAT] and mean annual precipitation minus potential evapotranspiration [MAP‐PET]), carbon (C) input (i.e., net primary production [NPP]), and soil property data synthesized from 72 published studies, along with data we generated from the National Ecological Observatory Network soil pits (n = 901 total observations). To assess the utility of investigating POC and MAOC separately in understanding SOC storage controls, we then compared these results with another path analysis predicting bulk SOC storage. We found that POC storage is negatively related to MAT and soil pH, while MAOC storage is positively related to NPP and MAP‐PET, but negatively related to soil % sand. Our path analysis predicting bulk SOC revealed similar trends but explained less variation in C storage than our POC and MAOC analyses. Given that temperature and pH impose constraints on microbial decomposition, this indicates that POC is primarily controlled by SOC loss processes. In contrast, strong relationships with variables related to plant productivity constraints, moisture, and mineral surface availability for sorption indicate that MAOC is primarily controlled by climate‐driven variations in C inputs to the soil, as well as C stabilization mechanisms. Altogether, these results demonstrate that global POC and MAOC storage are controlled by separate environmental variables, further justifying the need to quantify and model these C fractions separately to assess and forecast the responses of SOC storage to global change.