Nearly 20% of tropical forests are within 100 m of a nonforest edge, a consequence of rapid deforestation for agriculture. Despite widespread conversion, roughly 1.2 billion ha of tropical forest remain, constituting the largest terrestrial component of the global carbon budget. Effects of deforestation on carbon dynamics in remnant forests, and spatial variation in underlying changes in structure and function at the plant scale, remain highly uncertain. Using airborne imaging spectroscopy and light detection and ranging (LiDAR) data, we mapped and quantified changes in forest structure and foliar characteristics along forest/oil palm boundaries in Malaysian Borneo to understand spatial and temporal variation in the influence of edges on aboveground carbon and associated changes in ecosystem structure and function. We uncovered declines in aboveground carbon averaging 22% along edges that extended over 100 m into the forest. Aboveground carbon losses were correlated with significant reductions in canopy height and leaf mass per area and increased foliar phosphorus, three plant traits related to light capture and growth. Carbon declines amplified with edge age. Our results indicate that carbon losses along forest edges can arise from multiple, distinct effects on canopy structure and function that vary with edge age and environmental conditions, pointing to a need for consideration of differences in ecosystem sensitivity when developing land-use and conservation strategies. Our findings reveal that, although edge effects on ecosystem structure and function vary, forests neighboring agricultural plantations are consistently vulnerable to long-lasting negative effects on fundamental ecosystem characteristics controlling primary productivity and carbon storage.