Developing highly active catalysts for bio-oil hydrodeoxygenation is of great importance in the low cost production of conventional transport alkane fuels. Toward this goal, a Ni catalyst supported on mesoporous ZSM-5 zeolite mixed with 25 wt% gamma-Al2O3 (Ni/Al-HMZSM-5) was designed for hydrodeoxygenation of phenol as model compound. For comparison, the catalytic activities of Ni catalysts on conventional microporous ZSM-5, mesoporous ZSM-5 and gamma-Al2O3 were also investigated. It was found that almost complete phenol conversion (99.6%) was achieved over the Ni/Al-HMZSM-5 catalyst along with a high cyclohexane selectivity (98.3%) under a relatively mild condition (170 A degrees C, 4 MPa H-2). The open mesopores, stronger acid sites and synergism effect of Bronsted and Lewis acidities are jointly responsible for the excellent hydrodeoxygenation performance. In addition, it was shown that the catalyst was recycled several times with little loss of activity and selectivity.