Fast charging lithium-ion batteries are increasingly limited by interfacial mechanical failure between electrodes and current collectors, which leads to contact degradation, impedance growth, and accelerated performance decay under repeated electrochemical cycling. This work reports a chemically continuous and mechanically adaptive current collector architecture that addresses this overlooked bottleneck through the integration of polymethyl methacrylate-grafted natural rubber (MG30) and multi-walled carbon nanotubes (MWCNTs). The polar polymethyl methacrylate (PMMA) segments promote induced dipole interactions with the nanotube network, enabling the formation of a homogeneous conductive framework that combines high electrical conductivity with mechanical compliance. More importantly, the use of MG30 as both the current-collector matrix and electrode binder establishes a chemically continuous interface across the electrode-collector junction, resulting in enhanced adhesion, reduced interfacial resistance, and improved tolerance to cycling-induced stress accumulation. Unlike conventional aluminum current collectors, the elastomeric architecture exhibits intrinsic resistance to fluoride-induced corrosion while maintaining structural integrity during long-term operation. Consequently, lithium iron phosphate (LiFePO₄, LFP)||Li cells deliver stable high-rate performance and exceptional cycling durability, sustaining 4000 cycles at 10 C and retaining 80.3% capacity after 2000 cycles. The architecture further demonstrates compatibility with high mass loading electrodes and flexible pouch-cell configurations.

Solid-state lithium metal batteries (SLMBs) require quasi solid polymer electrolytes (QSSPEs) with high ionic conductivity, interfacial stability, and oxidative resistance. In this study, a QSSPE membrane (MP46, MG₃₀:LiTFSI:succinonitrile=10:4:6 by weight) with a wide electrochemical window of 5.1 V is designed to address these challenges. Complementary infrared spectroscopy, small-angle X-ray scattering and electron microscopy analysis reveals a hierarchical ionic conductive network, comprising sphere-like nanostructures embedded in microphase-segregated architectures. This architecture enhances lithium-ion transport while maintaining mechanical integrity. The strong interfacial adhesion of MP46 with lithium metal supports stable lithium plating and stripping for over 800 h at 0.2 mA·cm^–2, mitigating dendrite formation. When paired with LiFePO₄ and LiCoO₂ cathodes, MP46 sustains prolonged cycling, with capacity retention of 80.1% after 1400 cycles at 2 C and 92.1% after 200 cycles at 4.5 V, respectively. Pouch-type cells further demonstrate mechanical flexibility and operational safety under deformation. These results indicate that MP46 enables stable high-energy-density SLMBs, providing insights into the design of next-generation polymer electrolytes.