The carbon footprint of lithium-ion battery (LIB) manufacturing is an emerging concern with the rapid expansion of LIBs into electric vehicles and large-scale energy storage systems. In this context, dry electrode processing, enabled by polytetrafluoroethylene (PTFE) binders, offers a solvent-free, energy-efficient alternative to conventional slurry-based fabrication methods. Moreover, the unique fibril morphology of PTFE supports high-mass-loading electrodes without sacrificing ion transport or rate capability. However, PTFE's low intrinsic adhesion compromises the mechanical integrity of dry-processed electrodes, hindering practical application. Herein, we introduce a surface modification strategy based on polydopamine–poly(acrylic acid) coatings on graphite, enabling in-situ crosslinking during dry-processed electrode fabrication. This approach enhances the electrode adhesion strength without degrading electrochemical performance. The crosslinked electrodes exhibit superior mechanical stability and retain 87.1% of their initial capacity after 500 cycles at 1 C (4.3 mA cm−2), demonstrating a scalable route to robust, high-performance dry-processed electrodes.