To overcome their intrinsic limitations, a promising strategy is to construct hybrids composed of cobalt-based species and carbon materials. 2D graphitic carbon (GC) matrix with large surface area, high electrical conductivity, and robust mechanical stability is an excellent candidate in this regard. [7] Beyond planar integrated hybrids, an encapsulated structure of metallic nanoparticles within GC layer can be very effective in tuning activity and improving durability. In this configuration, metal electrons would transfer to carbon, which creates rich reactive sites and tunes electronic properties of the carbon materials, consequently accelerating electron/charge transfer kinetics. [8][9][10][11] It should be emphasized that the effective charge transfer is achieved via the formation of strong bridged bonds, which are absent in conventional carbon hybrids. Typically, metal-organic frameworks (MOFs) are chosen as carbon source to build the encapsulated structures. Nonetheless, they still suffer from poor contact between carbon and metallic nanoparticles. [12] Moreover, the morphologies of MOF-derived carbon matrixes are limited largely to polyhedrons similar to that of the parent structures. [13] Thus, to introduce the bridged bonds and maximize the exposed active sites, structure and morphology of Co-based hybrids need to be rationally designed and achieved in a controlled manner. [14] In addition, synthetic route toward encapsulated structure with bridged bonds must be facile to realize scalable synthesis for practical application.Molten salt (MS) synthesis is a relatively simple and economical method to prepare various inorganic materials, in which MS is used as a reaction medium. For those solvent-based synthetic routes, solvation is a crucial step. However, molecular solvents hardly solvate inorganics like metals and oxides. The strong polarizing force of MSs can reduce the stabilization of metallic, ionic, or covalent bonds -a pool of ionized cations and anions. Thus, MS method is a powerful synthetic strategy allowing the access to a broad range of inorganic crystalline materials, as well as carbons. [15] Careful design of synthesis conditions (composition of molten salt, raw materials, etc.) can enable the regulation for the structure, morphology, and composition of the resulting material.Here, we designed a strongly coupled hybrid consisting of embedded cobalt oxide nanocrystals and encapsulated cobalt nanoparticles on graphitic carbon nanosheet (GCS), denoted as CoO x @GCS⊃Co, via a volatile organic salt-induced Strong coupling between non-noble metal and carbon materials that enables fast electrochemical reaction kinetics is highly desired in many energy-related applications. Herein, a volatile organic salt-induced heterogeneous molten salt method is proposed to couple embedded cobalt oxide nanocrystals and encapsulated cobalt nanoparticles on a 2D graphitic carbon matrix, featuring enhanced charge transport and increased exposed active sites. Originating from its unique structure, this hybrid delivers...