Updated project metadata. Soil microorganisms act as gatekeepers for soil-atmosphere carbon exchange by balancing the accumulation and release of soil organic matter. However, poor understanding of the mechanisms responsible hinders the development of effective land management strategies to enhance soil carbon storage. Here we empirically test the link between microbial ecophysiological traits and topsoil carbon content across geographically distributed soils and land use contrasts. We discovered distinct pH-controls on microbial mechanisms of carbon accumulation. Land use intensification in low-pH soils that increased pH above a threshold (~ 6.2) lead to carbon loss through increased decomposition following alleviation of acid-retardation of microbial growth. However, loss of carbon with intensification in near neutral-pH soils was linked to decreased microbial biomass and reduced growth efficiency that was, in turn, related to tradeoffs with stress alleviation and resource acquisition. Thus, less intensive management practices in near neutral-pH soils have more potential for carbon storage through increased microbial growth efficiency; whereas, in acidic soils microbial growth is a bigger constraint on decomposition rates.