The nanosheets of Co/Zn phosphate were deposited on nickel foam with the organized flower-like structure through a facile one-pot hydrothermal method. The resulted Co-Zn-P/NiFoam exhibits excellent electrocatalytic performance of oxygen evolution in basic solution and hydrogen evolution in acid solution with low onset potentials, high current responses, low Tafel slopes and good long-term stabilities. The nanosheet organized flower-like structure may contribute to the more active sites for target molecules, the higher efficiency for mass migration and electron transfer. The compact layer of Co/Zn phosphate may play a great role in its electrocatalytic stability for both OER in basic solution and HER in acid solution. This work offers a facile strategy to fabricate inexpensive and efficient electrocatalysts towards water splitting for possible applications in the future.