The synthesis of bis(5-methylfuran)methane (BMFM) from biomass-based 5-methylfurfural (5-MF), a vital fuel precursor, is crucial for biomass refining. However, selective BMFM production from 5-MF needs to suppress side reactions such as hydrogenolysis and decarbonylation. Therefore, direct hydrogenation of 5-MF into BMFM is very challenging in sustainable biomass valorization. In this study, we developed a bimetallic RuCu/hydroxyapatite (HAP) catalyst for selective synthesis of BMFM from 5-MF. The RuCu/HAP catalyst delivered a BMFM yield of 75.6% under mild reaction conditions (