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Solid-state electrolytes from S2−/Sn2− integrated polyvinylpyrrolidone (PVP) are synthesized by a simple blending method. The ionic conductivity, charge-transfer ability, and therefore photovoltaic performances are optimized by adjusting the Na2S/S stoichiometric ratio. The quantum dot-sensitized solar cell (QDSSC) is assembled by sandwiching the solid electrolyte between a CdS-sensitized TiO2 anode and a CoSe alloy counter electrode. An optimal efficiency of 0.55% is measured for the QDSSC employing PVP/10Na2S–S solid electrolyte. The present work demonstrates the feasibility of designing cost-effective solid-state electrolytes with PVP, and the photovoltaic performances of QDSSCs can be further elevated by optimizing the synthesis conditions.