This article focuses on the catalytic hydrodenitrogenation (HDN) mechanism of indole under hydrothermal conditions. Formic acid (FA), which is a donor of both gaseous hydrogen and liquid hydrogen, can improve indole conversion and total yield of denitrogenated products. Ru/C showed the highest activity among the catalysts in this study for indole conversion at all temperature conditions with the existence of H 2 , and 91.17% indole was converted at 400 C and 60 min. Based on reaction kinetic experiments, a kinetic model was developed mathematically to describe the hydrothermal HDN reaction of indole over the home-made Ni 80 Ru 20 /γ-Al 2 O 3 catalyst, which clearly captured all data trends and fitted the temporal variation of all major liquid products. High activation energy for the formation of the O-containing substance o-cresol from both mathematical fitting and density functional theory (DFT) calculation indicated the rare occurrence of a reaction between the pyrrole ringopening product methyl aniline and H 2 O, consistent with the experimental observation that only a trace of o-cresol was detected.