Here we show how increased bioenergy production can be targeted through changes in management of rainfed, temperate agriculture and forestry. Bioenergy production can be substantially increased with reduced environmental impacts and minor effects on food and feed production. Even though global net primary production (NPP) may constitute a planetary boundary for bioenergy production, we show that at regional scale NPP can be increased and the human appropriation hereof (HANPP) may be sustainably increased. If this biomass is used for bioenergy in the form of highly relevant energy carriers, greenhouse gas emissions can be significantly reduced.