Controlling the furfural reaction pathways is an important step toward valorizing this important platform chemical in biomass conversion. In this work, high resolution electron energy loss spectroscopy (HREELS) and temperature programmed desorption (TPD) are employed to directly study the correlations between furfural reaction pathways and interactions between furfural and different surfaces, including Fe(110), Ni(111), Cu(111) and Pt(111). Surfaces with strong interactions with the furan ring favor decomposition products, while surfaces with weak ring interactions lead to furan production. Oxophilic metal surface like Fe(110) promotes the hydrodeoxygenation pathway to produce 2-methylfuran due to strong interaction with the carbonyl group. These results should provide guidance in the catalyst design for converting furfural to value-added products.