Summary Plant ecologists use functional traits to describe how plants respond to and influence their environment. Reflectance spectroscopy can provide rapid, non‐destructive estimates of leaf traits, but it remains unclear whether general trait‐spectra models can yield accurate estimates across functional groups and ecosystems. We measured leaf spectra and 22 structural and chemical traits for nearly 2000 samples from 103 species. These samples span a large share of known trait variation and represent several functional groups and ecosystems, mainly in eastern Canada. We used partial least‐squares regression (PLSR) to build empirical models for estimating traits from spectra. Within the dataset, our PLSR models predicted traits such as leaf mass per area (LMA) and leaf dry matter content (LDMC) with high accuracy ( R 2 > 0.85; %RMSE < 10). Models for most chemical traits, including pigments, carbon fractions, and major nutrients, showed intermediate accuracy ( R 2 = 0.55–0.85; %RMSE = 12.7–19.1). Micronutrients such as Cu and Fe showed the poorest accuracy. In validation on external datasets, models for traits such as LMA and LDMC performed relatively well, while carbon fractions showed steep declines in accuracy. We provide models that produce fast, reliable estimates of several functional traits from leaf spectra. Our results reinforce the potential uses of spectroscopy in monitoring plant function around the world.