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The nickel‐iron based materials are widely studied as excellent oxygen evolution reaction (OER) electrocatalysts. However, its relatively poor OER stability limits its practical applications. Herein, a zipper‐like interlocked heterostructure of NiFe layered double hydroxide (LDH)‐WN is constructed. The NiFe LDH‐WN exhibits not only ultrahigh OER activity of 228 mV overpotential at a current density of 50 mA cm−2, but also extremely long‐term stability over 4500 h at 50 mA cm−2 and over 550 h at an industrial current density ≈350 mA cm−2, which is ascribed to its special zipper‐like interlocked structure. Moreover, in situ Raman confirms that the presence of WN can efficiently achieve NiFe LDH reconstruction to slower the metal dissolution during OER, and therefore boosts its stability. DFT calculations reveal that WN not only can increase the *O adsorption capability and conductivity of NiFe LDH layer, but also can anchor the metal atoms of NiFe LDH layer to improve the dissolution energy barrier. In short, this work presents a new method of constructing the interlocked heterostructure to improve the OER stability of Ni‐Fe‐based catalysts, which would accelerate its practical application. [ABSTRACT FROM AUTHOR]

Interface engineering shows distinct advantages in the electrocatalytic hydrogen evolution reaction (HER) due to the unique structures that can be realized. The interfaces formed by amorphous materials often exhibit special properties that are beneficial for the HER. Herein, an amorphous/crystalline Rh(OH)3/CoP heterostructure is constructed, which exhibits outstanding HER performance in the all‐pH range. It only needs the overpotentials of 13, 12, and 25 mV to drive a current density of 10 mA cm−2 in alkaline, acidic, and neutral media, respectively, which ranks as one of the best HER electrocatalysts reported recently. The outstanding HER activities in the all‐pH range are attributed to the unique amorphous/crystalline heterostructure of Rh(OH)3/CoP, which possesses special hydrophilic/aerophobic features thataccelerate mass transfer, and provide abundant exposed active sites and appropriate defects. Importantly, the performance attenuation mechanism of the catalyst is also revealed, i.e., the formation of Rh aggregations leads to poor contact and efficacy loss of the amorphous/crystalline interface for HER. In short, this work provides a new idea for using amorphous/crystalline heterostructure to design electrocatalysts, not only for the HER, but also for the oxygen reduction and oxygen evolution reactions. [ABSTRACT FROM AUTHOR]