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The effects of using CH₄ as an assistant reduction agent in plasma-assisted NH₃−SCR were investigated. The new hybrid reaction system performed better than DBD−NH₃−SCR when the O₂ concentration varied from 2% to 12%. Compared with DBD−NH₃−SCR, DBD−NH₃−CH₄−SCR (NH₃:CH₄ = 1:1) showed a more significant promotion effect on the performance and N₂ selectivity for NO_X abatement. When the O₂ concentration was 6% and the SIE was 512 J/L, the NO removal efficiency of the new hybrid system reached 84.5%. The outlet gas components were observed via FTIR to reveal the decomposition process and its mechanism. This work indicated that CH₄, as an assistant agent, enhances DBD−NH₃−SCR in excess oxygen to achieve a new process with significantly higher activity at a low temperature (≤348 K) for NO_X removal.