Magnesium hydride(MgH2),which possesses high hydrogen density of 7.6 wt％,abundant resource and non-toxicity,has captured intense attention as one of the potential hydrogen storage materials.However,the prac-tical application of Mg/MgH2 system is suffering from high thermal stability,sluggish absorption and desorption kinetics.Herein,two-dimensional(2D)vanadium nanosh-eets(VNS)were successfully prepared via a facile wet chemical ball milling method and proved to be highly effective on improving the hydrogen storage performance of MgH2.For instance,the MgH2+7 wt％VNS composite began to release hydrogen at 187.2℃,152℃lower than that of additive-free MgH2.At 300℃,6.3 wt％hydrogen was released from the MgH2+7 wt％VNS composite within 10 min.In addition,the fully dehydrogenated sample could absorb hydrogen even at room temperature under hydrogen pressure of 3.2 MPa.X-ray diffractometer(XRD)and transmission electron microscopy(TEM)results confirmed metallic vanadium served as catalytic unit for facilitating the de/rehydrogenation reaction of MgH2.This finding presents an example of facile synthesis of two-dimensional(2D)vanadium with excellent cataly-sis,which may shed light on future design and preparation of highly effective layered catalysts for hydrogen storage and other energy-related areas.