CdSxSe1−x films of different composition (0 < x < 1) were deposited by pulse plating technique at different duty cycles in the range of 10–50%. The films were polycrystalline and exhibited hexagonal structure. The band gap of the films varies from 1.68 to 2.39 eV as the concentration of CdS increases. Energy Dispersive analysis of X-rays (EDAX) measurements indicate that the composition of the films are nearly the same as that of the precursors considered for the deposition. Atomic force microscopy studies indicated that the grain size increased from 20 to 200 nm as the concentration of CdSe increased. Photoelectrochemical (PEC) cell studies indicated that the films of composition CdS0.9Se0.1 exhibited maximum photoactivity. Mott-Schottky studies indicated that the films exhibit n-type behaviour. Spectral response measurements indicated that the photocurrent maxima occurred at the wavelength value corresponding to the band gap of the films.