The technical feasibility of developing a novel process for coupling bioderived furans (furfural) with methane was investigated at mild reaction conditions (400 °C and 2.5 MPa) over modified zeolite catalysts. Monoaromatics are the main liquid products with high yield, and the oxygen of furfural is removed in the form of CO and CO2. Compared to other zeolite-supported metal catalysts developed in this study, Zn–Ga/ZSM5 shows better catalytic performance on furfural conversion in terms of a higher yield of aromatics, particularly benzene, toluene and xylene (BTX), slightly lower gas yield and higher methane conversion. The presence of methane provides carbon atoms that are effectively utilized in the formation of aromatics, and further significantly enhances the yield of aromatics under the facilitation of the charged catalyst. Direct evidence of methane participation in the formation of aromatic products is witnessed by liquid 1H, 2H and 13C NMR investigations, which reveal that methane tends to be incorp...