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The in situ growth of nano-array on material structure is a novel and high-efficient strategy to design catalysts,however,it still remains a challenge to fabricate unique nano-architecture electrocatalyst with prominent activity and superior durability for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER).Herein,a unique nano-architecture catalyst is successfully synthesized by using NiFe LDH nanosheets as framework to the in situ growth Mo-doped Ni2P ultrafine nanosheets (marked as Mo-Ni2P@NiFe LDH/NF).The unique 3D core-shell nano-architecture is favorable for enhancing electron transfer/mass diffusion,providing abundant active sites,prompting O2/H2 gas release,and creating the synergistic effect between Mo-Ni2P and NiFe LDH.Therefore,comparing with pure NiFe LDH/NF and MoNi2P/NF electrodes,walnut-like Mo-Ni2P@NiFe LDH/NF catalyst exhibits significantly improved electrocatalytic activities and durability towards OER (269 mV@40 mA cm-2),HER (82 mV@10 mA cm-2),and overall water splitting (1.46 V@10 mA cm-2),respectively.Such electrocatalytic activity of Mo-Ni2P@NiFe LDH/NF is comparable with that of majority reported non-precious metal catalysts and even precious catalysts (lrO2 and Pt/C).This work presents a new perspective strategy to fabricate ingeniously bifunctional electrocatalysts with well-designed structure and superior performance for clean energy conversion technologies or storage devices.