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Atomic non-noble metal materials show the potential to substitute noble metals in catalysis. Herein, melamine formaldehyde resin is developed to synthesize atomic iron on mesoporous nitrogen-doped carbon. The triazine units with abundant nitrogen content and cavity can realize effectively anchoring of single metal atoms. The atomic iron with unique charge and coordination characteristics shows superior catalytic performance in dehydrogenation reaction. Various N-heterocycles compounds and amines can be efficiently dehydrogenated into the corresponding products at room temperature, which is the mildest of all reported reaction conditions even when noble metal catalysts are considered. Therefore, development of atomic non-noble metal catalysts with mesoporous structure may provide an effective way to realize the substitution for noble metals in heterogeneous catalysis.