Hydrogen evolution reaction (HER) from water electrolysis is an ideal alternative solution to address the energy crisis and develop clean energy. However, the construction of an efficient electrocatalyst with multiple active sites that can ensure high metal utilization and promote reaction kinetics simultaneously still leaves a major challenge. Herein, we present a facile strategy to synthesize a HER catalyst comprising Pt single atoms (Pt) anchored in Fe vacancies and Pt quantum dots (Pt) on the surface of NiFe LDH. Benefitting from the hierarchical and ultrathin nanosheet arrays and strong electronic interaction between Pt/Pt and NiFe LDH matrix, the optimized sample (Pt-NiFe LDH) exhibits outstanding HER performance in 1 M KOH with ultra-low overpotentials of 20 and 67 mV at 10 and 100 mA cm, respectively, outperforming the benchmark Pt/C electrocatalyst. In addition, the electrolyzer using Pt-NiFe LDH as a cathode requires voltages of only 1.48 and 1.73 V to yield current densities of 10 and 1000 mA cm, respectively. The combination of in situ tests and density functional theory (DFT) calculations reveal that the synergy of Pt and Pt can optimize the kinetics of water dissociation and hydrogen desorption, thus the Volmer-Tafel pathway prevailing the HER process. This work provides a promising surface engineering strategy to develop catalysts for efficient and robust hydrogen evolution.