The large availability and renewable nature of lignin makes its upgrading to bioproducts of particular interest for sustainable development. The hydrodeoxygenation (HDO) of anisole specifically represents a model reaction for the conversion of lignin to biofuels through the removal of the aromatic carbon-oxygen bonds. To date, a range of Ni-based catalysts have been reported as highly active systems for the HDO of anisole. However, there has been a substantial lack of consideration given to the environmental characteristics of these catalytic systems, in contrast with the scope of the sustainable production of biofuels. Herein, Ni-based SiO2 catalysts are prepared by a solventless and highly efficient mechanochemistry approach, having a considerably lower environmental impact as compared to standard impregnation methods. Importantly, scrap catalytic converters (SCATs) are employed as co-catalysts, proving the possibility of enhancing the catalytic HDO of anisole, with a scarcely exploited waste material. The results demonstrate that the combined use of Ni/SiO2 as catalysts and Ni/SCATs as co-catalysts remarkably boosts the rate of the conversion of anisole up to more than 50% by achieving an almost complete conversion of anisole in only 40 min instead of at 200 °C and 4 MPa H2. © 2022 The Authors. Advanced Sustainable Systems published by Wiley-VCH GmbH.