The effect of chenodeoxycholic acid as the coadsorbent with a squaraine sensitizer on TiO2 nanocrystalline solar cells was investigated, and it was found that the coadsorbent prevents the squaraine sensitizer from aggregating on the TiO2 nanoparticles but reduces dye loading leading to an interdependent photovoltaic performance. Analysis of the absorption spectra, and incident monochromatic photon-to-current conversion efficiency data showed that the load of squaraine sensitizer as well as the appearance of H-aggregates is strongly dependent on the molar concentration of chenodeoxycholic acid coadsorbent. The open circuit voltage of the solar cells with chenodeoxycholic acid increases due to the enhanced electron lifetime in the TiO2 nanoparticles coupled with the band edge shift of TiO2 to negative potentials.