Precise design of low‐cost, efficient and definite electrocatalysts is the key to sustainable renewable energy. Herein, this work develops a targeted‐anchored and subsequent spontaneous‐redox strategy to synthesize nickel‐iron layered double hydroxide (LDH) nanosheets anchored with monodispersed platinum (Pt) sites (Pt@LDH). Intermediate metal‐organic frameworks (MOF)/LDH heterostructure not only provides numerous confine points to guarantee the stability of Pt sites, but also excites the spontaneous reduction for PtII. Electronic structure, charge transfer ability and reaction kinetics of Pt@LDH can be effectively facilitated by the monodispersed Pt moieties. As a result, the optimized Pt@LDH that with the 5% ultra‐low content Pt exhibits the significant increment in electrochemical water splitting performance in alkaline media, which only afford low overpotentials of 58 mV at 10 mA cm−2 for hydrogen evolution reaction (HER) and 239 mV at 10 mA cm−2 for oxygen evolution reaction (OER), respectively. In a real device, Pt@LDH can drive an overall water‐splitting at low cell voltage of 1.49 V at 10 mA cm−2, which can be superior to most reported similar LDH‐based catalysts. Moreover, the versatility of the method is extended to other MOF precursors and noble metals for the design of ultrathin LDH supported monodispersed noble metal electrocatalysts promoting research interest in material design.