Exploring economically efficient electrocatalysts with good electrocatalytic activity is essential for diverse electrochemical energy devices. Series of ultrathin metallic nickel-based holey nitride nanosheets were designed as bifunctional catalysts for the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER). They exhibit improved catalytic properties owing to the inherent advantages of their plentiful active reaction sites resulting from the complete exposure of the atoms in the large lateral surfaces and from the edges of pore areas, together with expanded lattice spacing distance. This obtained three-dimensional conductive integral architecture can not only accelerate the electron transportation by the highly orientated crystalline structure but also facilitate the diffusion of intermediate and gases. In terms of the OER electrocatalytic properties, a quite low overpotential (300 mV) is required for the holey two-dimensional (2D) Ni3Fe nitride nanosheets to deliver a current density of about 100 A g-1, with an enhanced improvement over IrO2by a factor of nearly 25 times. The holey 2D Ni3Fe nitride nanosheets also exhibit enhanced catalytic performance toward the HER, with a tiny overpotential (233 mV) to achieve a current density of about 100 A g-1with much better kinetic properties in comparison to those of highly active Pt/C.