Land-use change (LUC) has fundamentally altered the form and function of the terrestrial biosphere. Increasing human population, the drive for higher living standards, and the potential challenges of mitigating and adapting to global environmental change, mean that further changes in LUC are unavoidable. LUC has direct consequences on climate, via emissions of greenhouse gases and changing the surface energy balance, but also by affecting the emission of biogenic volatile organic compounds (BVOCs). Isoprenoids, which dominate global BVOC emissions, are highly reactive and strongly modify atmospheric composition. The effects of LUC on BVOC emissions and related atmospheric chemistry have been largely ignored so far. However, compared to natural ecosystems, most tree species used in bioenergy plantations are strong BVOC emitters, whereas intensively cultivated crops typically emit less BVOCs. Here we summarize the current knowledge on LUC-driven BVOC emissions and how these might affect atmospheric composition and climate. We further discuss land-management and plant-breeding strategies which could be taken to move towards climate-friendly BVOC emissions, whilst simultaneously maintaining or improving key ecosystem functions such as crop yield under a changing environment.