Multilayer Conductive Hybrid Nanosheets as Versatile Hybridization Matrices for Optimizing the Defect Structure, Structural Ordering, and Energy‐Functionality of Nanostructured Materials

The hybridization of conductive nanospecies has garnered significant research interest because of its high efficacy in improving the diverse functionalities of nanostructured materials. In this study, a novel synthetic strategy is developed to optimize the defect structure, structural ordering, and energy‐related functionality of nanostructured‐materials by employing a multilayer multicomponent two‐dimenstional (2D) graphene/metal oxide/graphene nanosheet (NS) as a versatile hybridization matrix. The hybridization of the robust trilayer, polydiallyldiammonium (PDDA)‐anchored reduced‐graphene oxide (prGO)/metal oxide/prGO NS effectively enhance the structural ordering and porosity of the hybridized MoS2/MnO2 NS through suppression of defect formation and tight stacking. In comparison with monolayer rGO/RuO2 NS‐based homologs, the 2D superlattice trilayer prGO/RuO2/prGO NS hybrids deliver better functionalities as a hydrogen evolution electrocatalyst and as a supercapacitor electrode, demonstrating the merits of hybridization with multilayer NSs. The advantages of using multilayer multicomponent conductive NSs as hybridization matrices arise from the enhancement of charge and mass transport through the layer flattening or defect suppression of the hybridized NSs and the increase in porosity, as evidenced by density functional theory calculations. Finally, the universal utility of multilayer NSs is confirmed by investigating the strong effect of the stacking order on the electrocatalytic functionality of MoS2/rGO/RuO2 films fabricated through layer‐by‐layer deposition. A new concept of synthetic strategy to improve various energy functionalities and mass/charge transports of nanostructured materials is developed by employing multilayer conductive graphene/inorganic/graphene nanosheet (NS) as an emerging versatile hybridization matrix. The universal usefulness of hybridization with multilayer multicomponent NSs in exploring high‐performance functional materials originates from optimization of the defect structure, structural ordering, and porosity of hybridized species.