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Quasi‐solid‐state polymer electrolytes are one of the most promising candidates for long‐life lithium‐metal batteries. However, introduction of plasticizers for high ion conductivity at room temperature inevitably gives rise to poor mechanical strength and requires a very thick electrolyte membrane, which is detrimental to safety and energy density of the batteries. Herein, inspired by tube brushes coupling hardness with softness, a novel superstructured polymer bottlebrush BC‐g‐PLiSTFSI‐b‐PEGM (BC = bacterial cellulose; PLiSTFSI = poly(lithium 4‐styrenesulfonyl‐(trifluoromethylsulfonyl) imide); PEGM = poly(diethylene glycol monomethyl ether methacrylate)) with a hard nanofibril backbone and soft functional polymer side‐chains is reported as an effective strategy to well balance the mechanical strength and ion conductivity of quasi‐solid‐state polymer electrolytes. The resulting single lithium‐ion conducting quasi‐solid‐state polymer‐brush electrolytes (SLIC‐QSPBEs) integrate the features of the ultrathin membrane thickness (10 µm), the nanofibril backbone‐strengthened porous nanonetwork (Young's modulus = 1.9 GPa), and the high‐rate single lithium‐ion conducting diblock copolymer brushes. As a result, the ultrathin yet robust SLIC‐QSPBEs enable ultralong‐term (over 3300 h) reversible and stable lithium plating/stripping in Li/Li symmetrical cell at a current density of 1 mA cm−2 for lithium anode. This work affords a promising strategy to develop advanced electrolytes for solid‐state lithium‐metal batteries.

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Hollow microporous organic nanospheres (H-MONs) are prepared by using polylactide-b-polystyrene diblock copolymers (PLA-b-PS) as the precursor via a hyper-cross-linking mediated self-assembly strategy, in which the hyper-cross-linking PS block forms the microporous organic shell framework, and the degradable PLA block produces the hollow mesoporous core structure. The formation mechanism, morphology, and porosity parameters of the resulting H-MONs are systematically investigated. Moreover, based on the hyper-cross-linking generated rigid microporous organic frameworks, hollow microporous carbon nanospheres (H-MCNs) can be achieved by further pyrolysis progress. The obtained H-MCNs as electrode materials of a supercapacitor exhibit excellent electrochemical performance with specific capacitances of up to 145 F g at 0.2 A g, with almost no capacitance loss even after 5000 cycles at 10 A g. More especially, H-MONs can be further act as "nanoreactors" for the synthesis of FeO nanoparticles within hollow cores to construct magnetic core-shell FeO@H-MONs nanocomposite materials. Our strategy represents a new avenue for the preparation of hollow morphology-controlled microporous organic polymers with various potential applications.

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