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• CoNi alloy encapsulated in N-doped thin graphene shell was synthesized from MOF. • One-pot cellulose conversion to γ-valerolactone using formic acid as hydrogen donor. • γ-Valerolactone yield reached as high as 55.9 % over AgPW/CoNi@NG. • Reaction mechanism of formic acid as hydrogen donor was revealed over CoNi@NG400. One-step efficient conversion of cellulose into value-added γ-valerolactone (GVL) is of great interest because it not only integrates complex tandem reactions in one-step, but also does not need additional hydrogen sources. To achieve this goal, it is crucial to fabricate high-performance catalyst that can accelerate both hydrolysis of cellulose and further transformation of generated stoichiometric levulinic acid (LA) and formic acid (FA) into GVL. CoNi nanoparticles encapsulated in N-doped thin graphene shell gave GVL yield as high as 55.9 % at 200 °C combined with Ag+-exchanged heteropolyacid (AgPW). This composite catalyst is highly resistant to the corrosion of LA and FA, and hence shows high catalytic stability. LA-adsorption FTIR spectra and DFT calculations indicate that LA and FA can penetrate through shell graphene layers into core CoNi sites via cracks. Compared to H 2 , FA can much more rapidly reduce LA because of its low dissociation energy barrier and high dissociation rate. [ABSTRACT FROM AUTHOR]