Abstract Detachable pressure sensitive adhesives (PSAs) show great potential in recycling the bonded components toward a circular economy, yet the existing challenges such as strict conditions, and time‐consuming, adhesive residues after detachment significantly hinder the developments and applications. Here, a pressure sensitive ionoadhesive (PSIA) tape is first designed that has excellent interfacial toughness to various substrates (≈1.8 kJ m −2 ) yet can be electrically detached with high efficiency under safe voltages (≥90% within 1 min). The unique properties are achieved by introducing liquid‐free lithium salt into poly(ionic liquids) to establish multiple non‐covalent interactions (NCIs) including strong electrostatic interactions, moderate lithium bonds, weak ion‐dipole interactions, and hydrogen bonding interactions. The multiple NCIs not only strengthen the physical crosslinking networks to improve the mechanical performances but promote the dissociation of lithium salt to improve the ion transport properties. Additionally, the elaborately designed low T g and intrinsic low modulus features endow the PSIA tape adhesion with excellent reworkability, recyclability, and re‐adhesion ability. It is believed this work offers a new strategy for designing electrically detachable and fully recyclable PSIA tapes, which facilitates the reuse and recycling of the bonded components and reduces industrial waste.