ABSTRACT: Thin films of CZTSSe with band gaps ranging from 1.0 to 1.6 eV have been deposited using a molecular-precursor approach in Aerosol Assisted Chemical Vapor Deposition (AACVD). The [S]:[Se] ratio has been varied and plays a key role in controlling the structure, morphology, electrical and optical properties of the deposited films. A Vegard-type analysis on the collected results showed a direct correlation between the concentration of selenium in the precursor mixture and key performance parameters of the deposited films.