Bioenergy can contribute to achieving European Union (EU) climate targets while mitigating impacts from current agricultural land use. A GIS-based modeling framework (1000 m resolution) is employed to match biomass supply (forest and agricultural residues, complemented by lignocellulosic energy crops where needed)with biomass demand for either electricity or bio-oil production on sites currently used for coal power in the EU-28, Norway, and Switzerland. The framework matches supply and demand based on minimizing the field-to-gate costs and is used to provide geographically explicit information on (i) plant-gate supply cost; (ii) CO2 savings;and (iii) potential mitigation opportunities for soil erosion, flooding, and eutrophication resulting from the introduction of energy crops on cropland. Converting all suitable coal power plants to biomass and assuming that biomass is sourced within a transport distance of 300 km, would produce an estimated 150 TW h biomass-derived electricity, using 1365 PJ biomass, including biomass from energy crops grown on 6 Mha. Using all existing coal power sites for bio-oil production in100-MW pyrolysis units could produce 820 PJ of bio-oil, using 1260 PJ biomass, including biomass from energy crops grown on 1.8 Mha. Using biomass to generate electricity would correspond to an emissions reduction of135 MtCO2, while using biomass to produce bio-oil to substitute for crude oil would correspond to a reduction of59 MtCO2. In addition, energy crops can have a positive effect on soil organic carbon in most of the analyzed countries. The mitigation opportunities investigated range from marginal to high depending on location.