Modified Ni/α-Al2O3 was investigated as a catalyst for partial oxidation of methane for syngas production at low temperature. Only Co-modified Ni/α-Al2O3 catalyst (Ni/Co/α-Al2O3) catalyzed the reaction below 673 K. 6.6 wt% Ni/3.6 wt% Co/α-Al2O3 catalyst showed the optimum balance of low reaction temperature and less carbon deposition. Structural analysis revealed close-contact or alloy structures between Ni and Co on Ni/Co/α-Al2O3 catalyst, which were crucial for low-temperature reaction. CH4/O2 pulse dosing test revealed that Co addition to Ni/α-Al2O3 catalyst improved CH4 combustion activity due to tolerance of oxidation.