Dry electrode processing has emerged as a promising technology for fabricating high-mass-loading electrodes owing to its solvent-free, simplified production. However, conventional polytetrafluoroethylene (PTFE) binders are limited by environmental concerns regarding per- and polyfluoroalkyl substances (PFAS). To address this, we present a PFAS-free bottlebrush binder synthesized via atom transfer radical polymerization (ATRP) and ring-opening metathesis polymerization (ROMP). Comprising poly(acrylic acid) (PAA) and poly(methyl acrylate) (PMA) side chains, it ensures adhesion and conductive additive affinity via hydrogen bonding and CH-π interactions. Notably, the unique bottlebrush polymer structure suppresses chain entanglement, lowering viscosity for enhanced processability. Consequently, robust dry electrodes were fabricated with minimal binder content, and superior adhesion and stable electrochemical performance were verified by mechanical and electrochemical tests.