AbstractReduced stomatal conductance is a common plant response to rising atmospheric CO₂ and increases water use efficiency (W). At the leaf-scale, W depends on water and nitrogen availability in addition to atmospheric CO₂. In hydroclimate models W is a key driver of rainfall, droughts, and streamflow extremes. We used global climate data to derive Aridity Indices (AI) for forests over the period 1965–2015 and synthesised those with data for nitrogen deposition and W derived from stable isotopes in tree rings. AI and atmospheric CO₂ account for most of the variance in W of trees across the globe, while cumulative nitrogen deposition has a significant effect only in regions without strong legacies of atmospheric pollution. The relation of aridity and W displays a clear discontinuity. W and AI are strongly related below a threshold value of AI ≈ 1 but are not related where AI > 1. Tree ring data emphasise that effective demarcation of water-limited from non-water-limited behaviour of stomata is critical to improving hydrological models that operate at regional to global scales.