Reducing overpotential and increasing current density remain a great challenge for promoting the application of transition metals-based layered double hydroxides (LDHs). Herein, Ni nanoparticles (similar to 10 nm) decorated NiFe LDH ultrathin (thickness: similar to 2 nm) nanosheets (Ni NP/NiFe LDH) were successfully synthesized which exhibited advanced electrocatalytic activity and long-term stability on both oxygen evolution reaction (OER) and urea oxidation reaction (UOR). The onset potentials for OER and UOR are 1.50 V and 1.34 V, respectively, both are lower than NiFe LDH under the same conditions. Moreover, the peak current density of UOR was 300 mA/cm(2), which is much larger than reported precious-metal free UOR catalysts. The excellent catalytic performance of Ni NP/NiFe LDH composite for OER and UOR is proposed to result from the abundant exposed active sites, small charge transfer resistance, and the synergistic effects between NiFe LDH and anchored Ni nanoparticles. This work provides inspiring ideas and helpful guidelines in design of low-cost but highly efficient electrochemical catalysts. (C) The Author(s) 2017. Published by ECS. All rights reserved.