The construction of active sites with excellent water oxidation activity is of great significance in the design of OER electrocatalysts. Herein, we propose an anion regulation strategy, in which N-doped carbon nanotubes play a protective role by coating the Ni3Fe alloy particles and two non-metallic elements S and Se are introduced to adjust the electronic structure, this can further help construct a heterogeneous surface, improve the valence state, and increase the hydrophilicity of the catalysts. The two as-prepared catalysts N-CNTs@NiS2/Fe7S8 (overpotential of 330 mV to achieve 50 mA cm-2 and Tafel slope of 51.49 mV dec-1) and N-CNTs@NiSe2/Fe3Se4 (360 mV and 72.32 mV dec-1, respectively) exhibited considerably high OER activity in 1.0 M KOH solutions.