Because of the environmental concerns about the use of fossil resources, it is imperative to explore renewable alternatives. Lignocellulose, an abundantly available biomass that avoids competition with the food industry, can be converted into sustainable aviation fuels and high-value chemicals through a process involving pyrolysis and hydrodeoxygenation (HDO). However, achieving commercial viability necessitates the development of highly efficient HDO catalysts and optimization of associated reaction conditions. This proposal centers on the design of innovative supported high-entropy alloys as catalysts for pyrolysis bio-oil HDO, focusing on enhancing catalytic activity, selectivity, and, most importantly, stability. Additionally, the project aims to map the effects of operating conditions on kinetics and unravel reaction mechanisms, with particular attention to understanding the impact of water as it is inherent to the bio-oil mixture to be hydrotreated. This understanding will provide vital insights for process optimization. Furthermore, the project aspires to bridge the gap between academic research and industrial application by investigating model components, multicomponent mixtures and authentic pyrolysis bio-oil feedstocks, and by elucidating disparities between gas and liquid phase operation.