Cadmium sulfide (CdS) thin films were deposited using chemical bath deposition (CBD) technique on fluorine-doped tin oxide glass substrates. Cadmium sulfate, thiourea, and ammonium hydroxide were used as Cd source, S source, and the complexing agent, respectively in the reaction bath. The post-deposition CdCl 2 activation of chemical bath deposited CdS (CBD-CdS) thin films was done by dip coating in a saturated CdCl 2 bath. X-ray diffractograms show the growth of large CdS grains with better crystalline quality over the recrystallization process due to CdCl 2 treatment. The development of large clusters was determined to be due to coalescence of smaller clusters. The photoelectrochemical (PEC) cell (CdS/Na 2 S 2 O 3 / Pt) parameters, such as V OC and I SC for CdCl 2 activated CBD-CdS thin films were found to be higher compared to untreated CBD-CdS thin films. The improved effective surface area of the film and higher carrier concentration due to grain boundary passivation could be the reason for higher V OC and I SC values found in CdCl 2 -treated CdS films. Additionally, all the CdCl 2 -treated CdS films showed an increase in the optical transmittance spectra and bandgap compared to untreated CdS films. Relative energy band edge position of the grown CdS films was found to be adjustable with the CdCl 2 treatment time. The best photoactivity was found for the CdS films which were dip-coated for 10 min in CdCl 2 solution.