<p>Poly(ionic liquid)s (PILs) are promising solid electrolytes because they simultaneously offer high ionic conductivity, chemical and electrochemical robustness, good mechanical strength, and facile processability. However, the covalent backbones of PILs preclude self-healing and closed-loop recycling, which increases their maintenance costs and environmental impact. Mimicking the reversible connectivity of neuronal synapses, this study introduces an ionic-liquid-based supramolecular polymer (ILSP) concept in which a multitopic ionic liquid is cross-linked through non-covalent interactions. Consequently, high ionic conductivity, spontaneous self-healing, and closed-loop recyclability are simultaneously achieved in a single solid electrolyte. As a proof-of-concept, dynamic Zr⁴⁺-COOH coordination between a carboxyl-terminated tetracationic ionic liquid and Zr⁴⁺ ions yields ILSP/Zr, a transparent and mechanically robust solid electrolyte that delivers an ionic conductivity of 1.29 × 10⁻² mS cm⁻¹ at 25 °C. Reversible metal-ligand interactions enable rapid damage healing even at −20 °C, and the ionic conductivity and healing efficiency of ILSP/Zr surpass those of reported lithium-salt-free self-healing PILs. Furthermore, acid-triggered depolymerization releases the ionic liquid monomer in a 90% yield, enabling closed-loop recycling. When deployed as an electrolyte, ILSP/Zr affords healable, recyclable all-solid-state electrochromic devices operable from −20 °C to 50 °C that retain &gt;99% of their electrochromic performance after five damage-heal cycles and five recycling cycles.</p>