The oxygen evolution reaction (OER), as a key half-reaction in water splitting for clean hydrogen energy, is kinetically sluggish and usually requires efficient electrocatalysts to reduce the overpotential. Herein, we report a simple method to synthesize novel two-dimensional Ni76Co24 layered double hydroxides (Ni76Co24-LDHs) nanosheets as an effective OER catalyst. The obtained Ni76Co24-LDHs display a low onset overpotential of 242 mV, along with an excellent cycling stability. The Tafel slope of Ni76Co24-LDHs is only 57 mV dec(-1) which demonstrates an active kinetics for OER. The high catalytic activity of Ni76Co24-LDHs may be attributed to the porous tremella-like structure with large surface area, synergistic effect of Ni and Co, and a pinning of the Co3+/4+ and Ni3+/4+. More importantly, the high catalytic property and simple synthetic method of Ni76Co24-LDHs may have a promising potential for practical application.