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Electrolyte active group (EAG) embedded structured hard segments have been developed via graphene oxide coupled with polyurethane chain. The polysulfide redox couples (S2-/S n 2-) free functionalized polyurethane electrolyte possesses electron donating pendant anions (carboxylate and sulfonate segments) with sufficient oxygenic functional groups on polyurethane backbone. Polyelectrolyte activity is due to elevation of number density of pendant anions (electrolyte active group) into polyurethane chain. Electrochemical impedance spectroscopy (EIS) reveals higher electrical conductivity (4.48 × 10−3 S/cm) for optimized PUI-GO (0.5 wt%) electrolyte. The electrolyte active groups are prone to facilitate photovoltaic reaction due to synergistic interaction and function with MPA capped CdS. The QDSSC (FTO-RGO/TiO 2 /MPA-CdS/PUI-GO/FTO-Pt) exhibits maximum power conversion efficiency (1.63 %) and open circuit potential (V OC = 0.594 V) under 1 sun (100 mW/cm2) photo illumination. V OC is found to be improved with PUI-GO electrolyte due to its multi-functional activities such as expanded electrocatalytic area, conducting nanochannel and interfacial passivation effect of carboxylate ion on photoanode. [Display omitted] • Tagging of graphene oxide within the polyurethane chain and subsequent functionalization to generate electrolyte active pendant anion suitable for photovoltaic redox reaction. • Preparation of MPA capped CdS quantum dot for the active material in solar cell. • Fabrication of solar cell using quantum dots and gel polyelectrolyte as hole transporting layer. • The resultant QDSSC exhibited open circuit potential (Voc = 0.594V) and photovoltaic conversion efficiency (η = 1.63%). [ABSTRACT FROM AUTHOR]