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The leaf nitrogen (N) and phosphorus (P) concentrations of terrestrial plants make large contributions to ecosystem function and dynamics. The relationship between aridity and leaf N and P has been established through experimental studies. However, few studies have focused on the large-scale effects of aridity on the leaf N and P of terrestrial plants. In this paper, we used linear regression models to test the effects of aridity on terrestrial plant leaf N and P and the N:P ratio based on global datasets. We found that aridity had significant effects on the leaf N and P and the N:P ratio of terrestrial plants. The strongest relationships were between fern leaf P, the fern N:P ratio, tree leaf P, the tree N:P ratio, vine leaf N, and the tree N:P ratio. Aridity could be used to predict the P and N:P ratio of terrestrial plants, particularly those of ferns and trees, on large scales in arid environments. Our study contributes to maintaining ecosystem functioning and services in arid environments under climate change.