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The polysulfide shuttle is a major challenge for practical application of lithium–sulfur (Li–S) batteries. To solve this issue, a thin layer (3 μm) of radially oriented 3D MoS2 nanospheres (3D MoS2) constructed by 2D MoS2 nanosheets is developed as an interlayer coating overlaid on the sulfur cathode, which can simultaneously prevent polysulfide migration and facilitate Li+ diffusion. The trapping and catalytic conversion of polysulfides would benefit from the abundant active edge sites and the large contact surface in the well-preserved MoS2 nanosheets. Meanwhile, fast Li+ diffusion can be realized by the expanded (002) interlayer of the MoS2 nanosheets along with the sufficient electrolyte wettability due to the open 3D structure. Thus, the Li–S batteries with a 3D MoS2 interlayer and the pure sulfur cathode exhibit high specific capacity, excellent cycling stability (62.5% capacity retention with a 0.06% capacity decay per cycle and >99% Coulombic efficiency over 600 cycles), and satisfactory areal capacities of 2.92–3.96 mAh cm–2 at different currents under increased sulfur loading. Furthermore, it is feasible to incorporate the slurry cast interlayer into the existing electrode fabrication, which sheds light on constructing advanced interlayers for commercially viable Li–S batteries.

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A bioinspired polymer-based nanocomposite consisting of hierarchically oriented 2D nanomaterials and polymers exhibits extraordinary properties in various applications. However, it is still a great challenge to break through the limitations of the fabrication process and polymer types for producing a laminated nanocomposite with no restrictions in dimension. Herein, large-area bulk polypropylene carbonate (PPC)/polytetrahydrofuran-functionalized reduced graphene oxide (PTHF-fRGO) nanocomposites with nacre-like layered structures are fabricated through a cost-effective and large-scale evaporation-induced self-assembly process, followed by thermal laminating. To enhance the interfacial compatibility and self-assembly efficiency, the 2D RGO are noncovalently functionalized via controlled termination of living PTHF. The comprehensive properties of the laminated composites, including thermal, mechanical, shape memory, and gas barrier properties, can be significantly improved by introducing highly oriented RGO (<5 wt %). Tuning the composition of oriented RGO (>5 wt %) and PPC matrix in the laminated nanocomposite yields a material with high thermal and electrical conductivities and electromagnetic interference (EMI) shielding properties. Thus, the resulting high-performance and multifunctional PPC-based materials with potential biodegradability are potential replacements for petroleum-based plastics in various applications.