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Herbivory and plant defenses exhibit a coupled decline along elevation gradients. However, the current ecological equilibrium could be disrupted under climate change, with a faster upward range shift of animals than plants. Here, we experimentally simulated this upward herbivore range shift by translocating low-elevation herbivore insects to alpine grasslands. We report that the introduction of novel herbivores and increased herbivory disrupted the vertical functional organization of the plant canopy. By feeding preferentially on alpine plants with functional traits matching their low-elevation host plants, herbivores reduced the biomass of dominant alpine plant species and favored encroachment of herbivore-resistant small-stature plant species, inflating species richness. Supplementing a direct effect of temperature, novel biotic interactions represent a neglected but major driver of ecosystem modifications under climate change. [ABSTRACT FROM AUTHOR]