In this work, the great performance of chitosan-based films blended with TiO2(CH/TiO2) is presented to adsorb the hazardous pollutant 2,4-dinitrophenol (DNP) from water. The DNP was successfully removed, with a high adsorption %: CH/TiO2exhibited a maximum adsorption capacity of 900 mg/g. For pursuing the proposed aim, UV–Vis spectroscopy was considered a powerful tool for monitoring the presence of DNP in purposely contaminated water. Swelling measurements were employed to infer more information about the interactions between chitosan and DNP, demonstrating the presence of electrostatic forces, deeply investigated by performing adsorption measurements by changing DNP solutions’ ionic strength and pH values. The thermodynamics, adsorption isotherms, and kinetics were also studied, suggesting the DNP adsorption’s heterogeneous character onto chitosan films. The applicability of pseudo-first- and pseudo-second-order kinetic equations confirmed the finding, further detailed by the Weber–Morris model. Finally, the adsorbent regeneration was exploited, and the possibility of inducing DNP desorption was investigated. For this purpose, suitable experiments were conducted using a saline solution that induced the DNP release, favoring the adsorbent reuse. In particular, 10 adsorption/desorption cycles were performed, evidencing the great ability of this material that does not lose its efficiency. As an alternative approach, the pollutant photodegradation by using Advanced Oxidation Processes, allowed by the presence of TiO2, was preliminary investigated, opening a novel horizon in the use of chitosan-based materials for environmental applications.