The invention provides a carbon species modified metal Ni-based catalyst and an application thereof. The catalyst comprises an oxide support, metal Ni supported on the oxide support and an N-containing organic carbon species, wherein the diameter of metal Ni particles is 12-18 nanometers; the N-containing carbon species is mainly attached to specific crystal faces of the metal Ni particles. The catalyst is prepared with the method comprising the following steps: 1) a solution A is obtained by dissolving a Ni-containing inorganic salt and an N-containing organic compound in deionized water; 2) solid oxide particles and the solution A are mixed in proportion, and then solid particles are obtained with a solvent evaporation method; 3) the solid particles are directly roasted at 500-600 DEG C, and NiO precursor particles are obtained; 4) the NiO precursor particles are activated in a hydrogen-containing atmosphere at 400-500 DEG C for 4-10 h, and the catalyst is obtained. The invention further provides an application of the carbon species modified metal Ni-based catalyst to a methanation reaction. The catalyst has good stability.