Leaf longevity (LL) varies more than 20-fold in tropical evergreen forests, but it remains unclear how to capture these variations using predictive models. Current theories of LL that are based on carbon optimisation principles are challenging to quantitatively assess because of uncertainty across species in the ‘ageing rate:’ the rate at which leaf photosynthetic capacity declines with age. Here, we present a meta-analysis of 49 species across temperate and tropical biomes, demonstrating that the ageing rate of photosynthetic capacity is positively correlated with the mass-based carboxylation rate of mature leaves. We assess an improved trait-driven carbon optimality model with in situ LL data for 105 species in two Panamanian forests. We show that our model explains over 40% of the cross-species variation in LL under contrasting light environment. Collectively, our results reveal how variation in LL emerges from carbon optimisation constrained by both leaf structural traits and abiotic environment.