In this report, we conducted the synthesis, fabrication, and characterization of chitosan-azobenzene films using the solvent evaporation method. The samples were characterized through thermogravimetric analysis, differential scanning calorimetry, contact angle measurements, atomic force microscopy, and ultraviolet-visible spectroscopy. The main goal of this study was to investigate the photoactivity of chitosan-azobenzene films utilizing LED light as a radiation source. Remarkably, employing both ultraviolet and visible light allowed us to witness the photoisomerization phenomenon of azobenzene, i.e., the direct process (trans -> cis), in the films. Moreover, we investigated the reverse process (cis -> trans) in the absence of light. Interestingly, this step can be executed in darkness, indicating zero energy demand for this phase of the process. The results indicated that these self-supporting materials are capable of harvesting and storing light energy.