The structural and optical properties of electrodeposited Cd1-xZnxS nanostructured thin films were investigated in the present paper for compositions of x = 0, 0.03, 0.06 and 0.09. X-ray diffraction patterns of the deposited thin films consisted of diffraction peaks related to cubic crystal lattice. The atomic compositional ratios were determined by performing energy dispersive spectroscopy measurements. Scanning electron microscopy images indicated that deposited thin films have nanostructured forms. Raman spectra of the Cd1-xZnxS thin films exhibited two vibrational modes associated with longitudinal optical mode and its first overtone. Transmission measurements were performed on the deposited thin films to get their band gap energies. It was seen from the analyses of absorption coefficient that band gap energy of Cd1-xZnxS thin films increases almost linearly from 2.40 to 2.51 eV as the composition was increased from x = 0 to x = 0.09.