This study reports a simple and low-cost method for water purification using recyclable natural fibers (coarse wool fibers) as column-filling media for adsorption in the dynamic mode. As an instance of a dissolved organic pollutant, a cationic dye (basic blue 9, BB9) was assayed. According to the Langmuir isotherm (recorded at 300 K), the calculated maximum adsorption capacity of the fibrous material was found to be 24.86 mg/g for the retention of BB9. Response surface methodology (RSM) was employed for the design of experiments and the model-based optimization of the adsorption process performed in the dynamic regime (fixed-bed column). The optimal conditions provided by RSM indicated an adsorbent column height of H = 13.5 cm and a feed flow rate of Fv = 3 mL/min; these operating parameters ensured a color removal efficiency of 92.56% after 240 min of contact time. The recorded breakthrough curve under the optimal conditions was further interpolated using five quantitative mathematical models (Adams–Bohart, Thomas, Yoon–Nelson, Yan, and Clark) to assess the dynamic behaviors in the fixed-bed column. The best goodness-of-fit was achieved for the Thomas and Yoon–Nelson models. Thus, the coarse wool fibers used in a fixed bed demonstrated a relevant efficiency in the removal of cationic organic pollutants from contaminated water.