• Leaf area (LA), mass per area (LMA), nitrogen per unit area (Narea) and the leaf-internal to ambient CO₂ ratio (χ) are fundamental traits for plant functional ecology and vegetation modelling. Here we aimed to assess how their variation, within and between species, tracks environmental gradients. • Measurements were made on 705 species from 116 sites within a broad north–south transect from tropical to temperate Australia. Trait responses to environment were quantified using multiple regression; within- and between-species responses were compared using analysis of covariance and trait-gradient analysis. • Leaf area, the leaf economics spectrum (indexed by LMA and Narea) and χ (from stable carbon isotope ratios) varied almost independently among species. Across sites, however, χ and LA increased with mean growing-season temperature (mGDD₀) and decreased with vapour pressure deficit (mVPD₀) and soil pH. LMA and Narea showed the reverse pattern. Climate responses agreed with expectations based on optimality principles. Within-species variability contributed < 10% to geographical variation in LA but > 90% for χ, with LMA and Narea intermediate. • These findings support the hypothesis that acclimation within individuals, adaptation within species and selection among species combine to create predictable relationships between traits and environment. However, the contribution of acclimation/adaptation vs species selection differs among traits.