A novel Nb 2 O 5 −ZrO 2 support was synthesized and used to support Ni or Mo metal as a catalyst, and γ-Al 2 O 3 and SAPO-11 were selected as supports for comparison. The catalysts were then used for catalytic hydrodeoxidation of glycerol trioleate (GT) and jatropha curcas oil into jetfuel-range hydrocarbons in one step. The results showed that the reduced Ni metal could significantly promote hydrodeoxidation of GT and improve the selectivity of alkanes (57.1−73.0%). The support had significant inference on the catalysts. The prepared Nb 2 O 5 −ZrO 2 support, due to its properties of high surface area (34.1 m 2 g −1 ), suitable pore size (13.7 nm), and appropriate medium-strength acidic sites with proper density, made the Ni/Nb 2 O 5 −ZrO 2 catalyst beneficial for the high selectivity of jet fuel (54.5%) in liquid products (68.5%). Ni/Nb 2 O 5 −ZrO 2 could reduce the generation of coke and gas and increase the yield of liquid product compared with Ni/ γ-Al 2 O 3 . On the other hand, Ni/Nb 2 O 5 −ZrO 2 had higher catalytic efficiency upon hydrodeoxidation of GT and could inhibit the excessive production of aromatics in liquid products compared with Ni/SAPO-11. In the final product of catalytic hydrocracking of GT over Ni/Nb 2 O 5 −ZrO 2 , the specific composition of hydrocarbons in the C8−C16 range was 65.9% alkanes, 8.6% aromatics, 16.1% olefins, and 2.3% oxygenates, indicating that the direct catalytic cracking product of GT over Ni/Nb 2 O 5 −ZrO 2 almost meets the needs of jet fuel.