<p>Recently, solar energy has received considerable momentum, predominantly in the dominance of its consistency in electricity. In a new generation, solar devices are fabricated by harnessing organic and inorganic materials to optimize their solar energy-capturing tendency. Among them, dye-sensitized solar cells (DSSC) have emerged as a fundamental device, showcasing for the first time how semiconductors, accompanied by organic and organometallic dyes, can enable solar energy conversion. However, a better way to create DSSC technology is backed by the progress of efficient perovskite solar cells, which show good solar energy conversion and long-lasting stability and reliability. However, DSSC offers unique advantages such as cost-effective production, flexibility, and appropriate suitability for wearable devices, which contribute to significant energy conversion efficiencies. This DSSC has shown vulnerability, including electrolyte volatilization and long-term operational stability, but its scientific values have declined. Thus, the scientific community has been ready to fabricate a quasi-solid electrolyte assembly. This review explores the use of biomaterials, specifically cellulose-based materials, as a replacement for traditional polymer electrolytes derived from petrochemicals. Cellulose emerges as an ideal candidate, permitting huge mechanical support and improving the redox couple’s functionality. When a DSSC device is fabricated using cellulose-based quasi-solid electrolytes, it addresses the key issues, including liquid electrolyte volatilization and long-term operational stability. This article advocates the incorporation of biomaterials for fabricating DSSC devices, highlighting their utility to boost efficiency and endorse environmental sustainability.</p>