The fabrication, thickness, and structure of aerogel films composed of covalently cross-linked cellulose nanocrystals (CNCs) and poly(oligoethylene glycol methacrylate) (POEGMA) were optimized for use as electrolyte absorbers in dye-sensitized solar cells (DSSCs). The aerogel films were cast directly on transparent conducting counter electrode substrates (glass and flexible poly(ethylene terephthalate) plastic) and then used to absorb drop-cast liquid electrolyte, thus providing an alternative method of filling electrolyte in DSSCs. This approach eliminates the use of electrolyte-filling holes, which are a typical pathway of electrolyte leakage, and furthermore enables a homogeneous distribution of electrolyte components within the photoelectrode. Unlike typical in situ electrolyte gelation approaches, the phase inversion method used here results in a highly porous (>99%) electrolyte scaffold with excellent ionic conductivity and interfacial properties. DSSCs prepared with CNC-POEGMA aerogels reached similar power conversion efficiencies as compared to liquid electrolyte devices, indicating that the aerogel does not interfere with the operation of the device. These aerogels retain their structural integrity upon bending, which is critical for their application in flexible devices. Furthermore, the aerogels demonstrate impressive chemical and mechanical stability in typical electrolyte solvents because of their stable covalent cross-linking. Overall, this work demonstrates that the DSSC fabrication process can be simplified and made more easily upscalable by taking advantage of CNCs, being an abundant and sustainable bio-based material.