The invention provides a kind of N, S co-doped graphene / MoSe 2 The preparation method of / CoFe-LDH airgel is characterized in that, comprises the following steps: S1, prepare graphene oxide lamellar dispersion liquid, MoSe respectively 2 Nanosheet dispersion and layered CoFe-LDH nanosheet dispersion; S2, the graphene oxide sheet dispersion and MoSe 2 Mix the nanosheet dispersion, add reducing agent and crosslinking agent, mix evenly, and react to prepare N, S co-doped graphene / MoSe 2 Hydrogel, freeze-dried to obtain N,S co-doped graphene / MoSe 2 Airgel; S3, the N,S co-doped graphene / MoSe 2 Airgel soaked in layered CoFe‑LDH nanosheet dispersion for N,S co-doped graphene / MoSe 2 / CoFe‑LDH hydrogel, freeze-dried N, S co-doped graphene / MoSe 2 / CoFe‑LDH airgel. Ternary N, S co-doped graphene / MoSe prepared by the present invention 2 / CoFe‑LDH airgel has better hydrogen evolution and oxygen evolution performance under alkaline conditions.