Low-surface-energy (LSE) materials, such as polytetrafluoroethylene (PTFE), are widely used in industrial applications, due to their exceptional hydrophobicity and chemical inertness. However, achieving strong adhesion to these materials has long posed a significant challenge. In this study, a high-performance adhesive is introduced that successfully overcomes this barrier, achieving an unprecedented bonding strength of up to 3.22 MPa on LSE substrates, the highest reported to date. This breakthrough is attributed to the synergistic effects of dipole–dipole interactions and frictional energy dissipation from the polymer side chains. By employing monomers with pendant side chains, such as poly(propylene glycol) methacrylate (PPGMA), both adhesion and toughness are enhanced without requiring any surface treatments. This adhesive exhibits remarkable versatility, effectively bonding to a variety of substrates, including PTFE, polypropylene (PP), polyethylene (PE), glass, ceramics, and steel. With a simple formulation, straightforward polymerization process, and high optical clarity, this adhesive presents a cost-effective solution with significant potential for diverse industrial applications.