<p>Dry electrode technology enables the fabrication of thick, low-cost electrodes by eliminating solvent processing, significantly improving battery energy density for scalable production. However, conventional aluminum (Al) current collectors suffer from insufficient interfacial bonding energy with dry electrodes, leading to delamination issues. This problem is exacerbated under high current densities, where Al corrosion accelerates interfacial contact failure, dramatically increasing interfacial resistance and degrading battery performance. To address this challenge, we propose an interfacial carboxyl network strategy by introducing high-density carboxyl functional groups on Al current collectors. Carboxyl functional groups form hydrogen bonding with the hydroxyl groups in the aluminum oxide (Al₂O₃) layer on the surface of the Al current collector, while their hydrogen atoms also engage in hydrogen bonding with fluorine atoms in the polytetrafluoroethylene (PTFE) binder, substantially enhancing electrode-current collector adhesion. Simultaneously, the dense carboxyl network passivates the collector surface and blocks electrolyte penetration, effectively inhibiting Al corrosion. As a proof-of-concept, a polyacrylic acid (PAA)-citric acid (CA)-carbon nanotubes (CNTs) composite conductive coating was constructed on Al current collectors. This design maintains structural integrity at ∼5000 Pa interfacial pressure while suppressing electrolyte corrosion. Even with a high areal mass loading of ∼30 mg cm⁻², the assembled Li∥NCM811 cell still can deliver a high discharge capacity of 201.4 mAh g⁻¹ at 13.9 mA g⁻¹. This work provides a crucial technical pathway for developing high-loading, high-energy-density lithium metal batteries.</p>