Negative emission technologies such as bioenergy with carbon capture and storage (BECCS) are regarded as an option to achieve the climatic target of the Paris Agreement. However, our understanding of the realistic sustainable feasibility of the global lands for BECCS remains uncertain. In this study, we assess the impact of BECCS deployment scenarios on the land systems including land use, water resources, and ecosystem services. Specifically, we assess three land-use scenarios to achieve the total amount of 3.3 GtC year⁻¹ (annual negative emission level required for IPCC-RCP 2.6) emission reduction by growing bioenergy crops which requires huge use of global agricultural and forest lands and water. Our study shows that (1) vast conversion of food cropland into rainfed bio-crop cultivation yields a considerable loss of food production that may not be tolerable considering the population increase in the future. (2) When irrigation is applied to bio-crop production, the bioenergy crop productivity is enhanced. This suppresses the necessary area for bio-crop production to half, and saves the land for agricultural productions. However, water consumption is doubled and this may exacerbate global water stress. (3) If conversion of forest land for bioenergy crop cultivation is allowed without protecting the natural forests, large areas of tropical forest could be used for bioenergy crop production. Forest biomass and soil carbon stocks are reduced, implying degradation of the climate regulation and other ecosystem services. These results suggest that without a careful consideration of the land use for bioenergy crop production, a large-scale implementation of BECCS could negatively impact food, water and ecosystem services that are supporting fundamental human sustainability.