In this work, we demonstrate the use of covalently linked CNC−POEGMA aerogel films as electrolyte absorbing “sponges” for the fabrication of DSSCs. Compared to previously reported methods, the current approach allows easy control of the aerogel density, composition, and final aerogel thickness. Furthermore, we show that due to the hydrazone cross-linking chemistry, these aerogels are very stable in ACN and 3-MPN, the two most commonly used solvents for DSSC electrolyte systems. The DSSC devices prepared from 10 and 44 μm thick aerogels yielded similar performance and stability as compared to nonaerogel- containing DSSCs, thus indicating that the used aerogel sponges do not interfere with the electrochemistry inside the device while also improving the ease of the DSSC device fabrication. This fabrication method can also be directly applied to flexible ITO−PET substrate, thus facilitating the production and upscaling of the device size for both glass- based and flexible DSSCs.