As renewable energy sources strive to match growing energy demands, new materials and designs constantly push the performance of preexisting solar cells to new levels. However complex patterning techniques or use of environmentally toxic materials limit the extent to which state-of-the-art designs can transition from research scale devices into commercially applicable devices. Biohybrid solar cells address this limitation by employing naturally occurring dyes or light harvesting protein complexes, such as photosystem I (PSI) in their design. In this work, multi-walled carbon nanotube (MWCNT)-coated electrodes have been modified with PSI to serve as high surface area anodes in an effort to enhance generated photocurrent. The chemical treatment of MWCNTs prior to deposition on conductive substrates resulted in uniform films and lead to a 7-fold enhancement in observed photocurrent compared to PSI-based devices assembled on unmodified, planar gold electrodes. This facile treatment and deposition of MWCNTs promotes their use in electrochemical devices as an inexpensive, robust, and high surface area alternative to other carbon allotropes.