Molybdenum supported on carbon nanotubes (CNTs) was synthesized and evaluated as a catalyst for the catalytic hydroprocessing of anisole. The CNTs and supported catalysts were characterized by X-ray diffraction crystallography, scanning electron microscopy, energy-dispersive X-ray spectroscopy, and surface area/pore volume measurements. The anisole conversion products and selectivity-conversion data led to the identification of kinetically significant reaction routes, hydrodeoxygenation (HDO) and hydrogenolysis, accompanied by some alkylation, and transalkylation; for example, including anisole conversion to benzene by HDO and to phenol by hydrogenolysis, and formation of methyl-substituted phenols by transalkylation and alkylation. The activity and selectivity of the CNT-supported catalyst compare favorably with those of comparable catalysts on other supports, but the molybdenum in the carbon nanotubes limits the access of reactants to the catalytically active molybdenum species.