A potentially appealing alternative to the traditional fabrication process of TiO2 film electrodes for dye-sensitized solar cells (DSSCs) was presented by utilizing water-soluble TiO2 composite pastes containing size-controlled ink particles (SIPs) isolated from the squid. The mixture ratios of SIPs in the paste formulations affected the photoelectric conversion efficiency (PCE). The highest PCE was achieved when the mixture ratio of SIPs was 20%. The process is highly reproducible and leads to a 35% increase in PCE compared with that in the DSSC without SIP addition. The utilization of SIPs in the fabrication of TiO2 film electrodes enhanced the performance of DSSCs.