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Heterostructures with interfacial effects have exhibited great potential for improving the electrochemical kinetics of electrode materials. However, the application of heterostructures is hampered by complicated synthesis parameters and numerous single components. Herein, a multiple‐templating synthesis strategy is proposed to improve the interfacial effect of heterojunction composites, mitigate volume variation upon lithiation/de‐lithiation, and increase interfacial compatibility with poly‐oxyethylene‐based (PEO‐based) electrolytes. Benefiting from the structural and compositional superiorities, the novel NiS/SnO2/MOF (NSM) electrode achieves superior electrochemical performance with exceptional specific capacity, outstanding rate capability and ultralong cyclability. As a result of the compatibility between organic components and the porous properties of metal organic frameworks (MOFs), the NSM electrode exhibits greater interfacial compatibility with PEO‐based solid‐state electrolytes. This work not only describes a meticulous protocol for heterostructured high‐performance electrode materials, but also provides a new insight to enhance the connectivity between the interfaces of solid‐state batteries. [ABSTRACT FROM AUTHOR]

Due to the excellent specific capacity and high working voltage, manganese oxide (MnO2) has attracted considerable attention for aqueous zinc‐ion batteries (AZIBs). However, the irreversible structural collapse and sluggish ionic diffusion lead to poor rate capability and inferior lifespan. Herein, we proposed a novel organic/inorganic hybrid cathode of carbon‐based poly(4,4′‐oxybisbenzenamine)/MnO2 (denoted as C@PODA/MnO2) for AZIBs. Various in/ex situ analyses and theoretical calculations prove that PODA chains with C=N groups can provide a more active surface/interface for ion/electron mobility and zinc ion storage in the hybrid cathode. More importantly, newly formed Mn−N interfacial bonds can effectively promote ion diffusion and prevent Mn atoms dissolution, enhancing redox kinetics and structural integrity of MnO2. Accordingly, C@PODA/MnO2 cathode exhibits high capacity (321 mAh g−1 or 1.7 mAh cm−2 at 0.1 A g−1), superior rate performance (88 mAh g−1 at 10 A g−1) and excellent cycling stability over 2000 cycles. Hence, rational interfacial designs shed light on the development of organic/inorganic cathodes for advanced AZIBs. [ABSTRACT FROM AUTHOR]