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Highlights: Face-to-face covalent bridging in-between 2D-nanosheets/graphene heterostructure was constructed by intentionally prebonding of laser-manufactured amorphous and metastable nanoparticles on graphene. The consecutive bonding enables the robust anchoring of ultrathin SnS2 nanosheets on graphene with huge covalent coupling area as well as spontaneous charge transfer in-between the heterostructure. Such laser-manufactured heterostructure is capable of guaranteeing high-flux electron/ion migration and structural integrity upon cycling, thus contributing to the unprecedented Na-storage capability. Establishing covalent heterointerfaces with face-to-face contact is promising for advanced energy storage, while challenge remains on how to inhibit the anisotropic growth of nucleated crystals on the matrix. Herein, face-to-face covalent bridging in-between the 2D-nanosheets/graphene heterostructure is constructed by intentionally prebonding of laser-manufactured amorphous and metastable nanoparticles on graphene, where the amorphous nanoparticles were designed via the competitive oxidation of Sn-O and Sn-S bonds, and metastable feature was employed to facilitate the formation of the C-S-Sn covalent bonding in-between the heterostructure. The face-to-face bridging of ultrathin SnS2 nanosheets on graphene enables the heterostructure huge covalent coupling area and high loading and thus renders unimpeded electron/ion transfer pathways and indestructible electrode structure, and impressive reversible capacity and rate capability for sodium-ion batteries, which rank among the top in records of the SnS2-based anodes. Present work thus provides an alternative of constructing heterostructures with planar interfaces for electrochemical energy storage and even beyond. [ABSTRACT FROM AUTHOR]

Robust anchoring of high‐capacity nanocrystals (NCs) on porous conductive substrates is of paramount importance but it is challenging for highly efficient energy storage to prevent the weak interfacial interactions, inevitable aggregation, and sluggish charge transfer, due to the technical hurdles of constructing heterostructures with firm electron/ion bridging. Herein, a facile and high‐efficiency liquid‐phase laser manufacturing strategy to guarantee the covalent bonding of ultrafine NCs on conductive substrates by predesigning metastable supranano (<10 nm) particles is proposed. The manufacturing of supranano SnO2 (≈3.4 nm) is demonstrated to tightly anchor on mesoporous walls of graphene with high loading (≈81.3%) and homogenous dispersion. Such a optimized heterostructure with unimpeded electron/ion transfer delivers extraordinary long‐term cycling stability (1132 mAh g–1 at 1.0 A g–1 after 1250 cycles) and impressive rate capability (275 mAh g–1 at 30.0 A g–1) as the anode for Li‐storage, which are some of the highest values among the reported SnO2‐based anodes. The study provides an important avenue for addressing the interfacial bridging in‐between heterostructures via creating active metastable supranano particles for intriguing electrochemical applications or even beyond, based on laser‐matter interactions. [ABSTRACT FROM AUTHOR]