Aqueous rechargeable zinc-ion batteries (ARZBs) have been intriguing for electrochemical energy storage applications because of their safety and cost-effectiveness. Regarding cathode materials, rapid development has been observed with the organic-based cathode materials that offer much higher structural integrity upon successive (de-)insertion of charge carries ions. Even though promising results demonstrated with organic electrodes, they still suffer from the short cycle-life due to their discharge products solubility in electrolyte. Herein, electrochemical performance and charge storage mechanism of the synthesized polyphosphazene-based inorganic-organic hybrid electrode containing pyrene-4,5,9,10-tetraone (PTO) redox active lateral group, poly[(bis(2-amino-4,5,9,10-pyrenetetraone)], abbreviated as (PPAPT), were investigated in ARZBs. The charge storage mechanism of PPAPT was examined by various ex-situ (Fourier Transform Infrared Spectroscopy (FTIR), X-ray Diffraction (XRD), Scanning Electron Microscopy and Energy Dispersive X-ray Spectroscopy (SEM-EDS), X-ray Photoelectron Spectroscopy (XPS)) and in-situ (pH change with bromocresol green indicator and Electrochemical Quartz Crystal Microbalance (EQCM)) characterization techniques as well as computational Density functional theory (DFT) revealing that the PPAPT electrode (de-)coordinates both zinc and proton. The electrode and its discharge product are insoluble in the electrolyte demonstrated by UV-vis analysis and exhibited a stable cycling performance with a discharge capacity of 125.4 mAh g-1 after 1000 cycles at a current density of 10 C.