Low-surface-energy (LSE) materials, such as polytetrafluoroethylene (PTFE), are extensively used in advanced technologies like 5G chip production and base station filters, due to their hydrophobicity, chemical resistance, low friction, and excellent dielectric properties. However, their inherent chemical inertness and nonwetting nature pose significant challenges to achieving strong adhesion. In this work, we present a pressure-sensitive adhesive (PSA) tape composed of fluorinated monomers and hydrophobic ionic liquids, synthesized through a one-step, scalable process. This adhesive demonstrates an impressive bond strength of 1700 N/m on PTFE, significantly outperforming existing adhesives for LSE substrates. The enhancement arises from the strategic incorporation of ion-dipole interactions between the polar -CF3 groups in the fluorinated monomers and the ionic liquid cations, which create sacrificial bonds to improve cohesion and energy dissipation. Remarkably, this adhesive requires no surface pretreatment, maintains high transparency, and demonstrates stable adhesion even under high humidity. This work addresses a critical gap in adhesion technology for LSE materials, offering a scalable and versatile solution with diverse applications in advanced electronics, aerospace, and other industries demanding high-performance adhesives.