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Bioenergy represents the highest share of renewable energies consumed in the European Union and is still expected to grow. This could be possible by exploring bioenergy production on Marginal, Underutilised, and Contaminated lands (MUC) that are not used for agricultural purposes and therefore, present no competition with food/feed production. In this paper, the viability and sustainability of bioenergy value chains on these lands is investigated and measures for market uptake were developed. Using three case study areas in Italy, Ukraine, and Germany, a screening of MUC lands was conducted, then an agronomic assessment was performed to determine the most promising crops. Then, techno-economic assessments followed by sustainability assessments were performed on selected value chains. This concept was then automated and expanded through the development of a webGIS tool. The tool is an online platform that allows users to locate MUC lands in Europe, to define a value chain through the selection of bioenergy crops and pathways, and to conduct sustainability assessments measuring a set of environmental, social, and economic sustainability indicators. The findings showed positive results in terms of profitability and greenhouse gas emissions for bioethanol production from willow in Ukraine, heat and power production from miscanthus, and biogas and chemicals production from grass in Germany. The webGIS tool is considered an important decision-making tool for stakeholders, which gives first insights on the viability and sustainability of bioenergy value chains. [ABSTRACT FROM AUTHOR]