In an effort to explore the optoelectronic properties of nanostructured indium sulfide (In2S3) thin films for a wide range of applications, the In2S3 thin films were successfully deposited on the APTS layers (–NH2-terminated) modified ITO glass substrates using the chemical bath deposition technique. The surface morphology, structure and composition of the resultant In2S3 thin films were characterized by FESEM, XRD, and XPS, respectively. Also, the correlations between the optical properties, photocurrent response and the thickness of thin films were established. According to the different deposition mechanisms on the varying SAMs terminational groups, the positive and negative micropatterned In2S3 thin films were successfully fabricated on modified Si substrates surface combining with the ultraviolet lithography process. This offers an attractive opportunity to fabricate patterned In2S3 thin films for controlling the spatial positioning of functional materials in microsystems.