Significance Ecology seeks general principles describing how the biota respond to multiple environmental factors, partly to build a more prognostic science in the face of global climate change. One such principle to emerge is the “leaf economics spectrum” (LES), which relates ecologically important plant nutrients to leaf construction and growth along simple relational axes. However, interrelationships between LES traits have not been tested at large geographic scales. Using airborne imaging spectroscopy and geospatial modeling, we discovered strong climatic and geophysical controls on LES traits and their interrelationships throughout Andean and western Amazonian forest canopies. This finding highlights the need for biogeographically explicit treatment of plant traits, afforded by imaging spectroscopy, in the next generation of biospheric models.