Potassium (K) is the second most abundant nutrient element in plants after nitrogen (N), and has been shown to limit aboveground production in some contexts. However, the role of N and phosphorus (P) availability in mediating K limitation in terrestrial production remains poorly understood; and it is unknown whether K also limits belowground carbon (C) stocks, which contain at least three times more C than those aboveground stocks. By synthesizing 779 global paired observations (528, 125, and 126 for aboveground productivity, root biomass, and soil organic C [SOC], respectively), we found that K addition significantly increased aboveground production and SOC by 8% and 5%, respectively, but did not significantly affect root biomass (+9%). Moreover, enhanced N and/or P availability (through N and P addition) did not further amplify the positive effect of K on aboveground productivity. In other words, K had a positive effect on aboveground productivity only when N and/or P were limiting, indicating that K could somehow substitute for N or P when they were limiting. Climate variables mostly explained the variations in K effects; specifically, stronger positive responses of aboveground productivity and SOC to K were found in regions with high mean annual temperature and wetness. Our results suggest that K addition enhances C sequestration by increasing both aboveground productivity and SOC, contributing to climate mitigation, but the positive effects of K on terrestrial C stocks are not further amplified when N and P limitations are alleviated.