Ionoadhesives show great potential for the electrical detachment of structural bonds due to the rapid interfacial electrochemistry reactions (IERs) of ion carriers, but previous ionoadhesives suffer from liquid leakage or contradictory mechanical performances and ion transport properties. Here, we introduce a charge delocalization strategy to simultaneously improve the mechanical performances and ion transport properties of poly(ionic liquid) ionoadhesives (PIAs). In addition, charge delocalization sharply decreases the escaping energy of mobile ions and thus significantly facilitates ion hopping. Consequently, a liquid-free PIA with outstanding bonding strength, toughness, dynamic stability, and ionic conductivity is presented. Moreover, the occurrence of rapid IERs under direct current (DC) voltages endows high-strength PIAs with outstanding electrical detachment behavior (complete detach within 1 min). This work creates a new opportunity to balance the mechanical performances and ion transport properties of ionic conductive materials, and the resulting electrically detachable PIAs demonstrate a significant role in circular economy.