In future biorefineries, the development of cheap and environmentally friendly solvents for biomass pretreatment is highly desirable. In this sense, low-transition-temperature mixtures (LTTMs) have high potential to serve as green solvents for replacing conventional pretreatment technologies. In this study, a life cycle assessment of LTTMs pretreatment was conducted to determine the environmental impacts caused by biomass delignification. A gate-to-gate analysis which started with harvested oil palm empty fruit bunch and ended with lignin was selected. The environmental impacts such as acidification potential, global warming potential, eutrophication potential, photochemical ozone creation potential, human toxicity potential and volatile organic compounds emission were evaluated. The comparable environmental balances of commercial l-malic acid and cactus malic acid-based LTTMs pretreatment processes verified the suitability of the process with natural malic acid as the source of proton donor. This study concludes that biomass delignification using natural cactus malic acid-based LTTMs had promising features such as high delignification efficiency and environmentally friendly compared to commercial l-malic acid-based LTTMs. Based on environmental point of view, the overall process of biomass delignification using sucrose-based LTTMs had lower CO2 emissions compared to the monosodium glutamate- and choline chloride-based LTTMs. These findings are important for verifying the greenness and sustainability of LTTMs to be applied at industrial scale. © 2018, Springer-Verlag GmbH Germany, part of Springer Nature.