In this work, Azolla filiculoides was used for the bioremediation of a textile effluent and as a potential sorbent for the rejection of Congo red (CR9) dye from a synthetic aqueous solution. The sorbent was characterized, and a pot culture test was carried out to assess the physiological responses in a controlled environment. The response of the plants to the exposure to the emanating pollutants was subordinate. The BOD, COD, and TDS removals were found to be 98.2%, 98.23%, and 90.29%, respectively. Moreover, the dried biomass was studied for the expulsion of CR9, and the process variables were optimized. The maximum CR9 removal was 95% at the optimal conditions of 2 g/L of the sorbent dose at acidic pH. Equilibrium data for adsorption were analyzed using a two-parameter isotherm model. It was observed that the Langmuir isotherm fit with the data (R2 = 0.98) and also had satisfactory lower error values, with its maximum sorption capacity reaching 243 mg/g. The pseudo-second-order kinetics were well fitted (R2 = 0.98). The mass transfer models and the thermodynamic parameters of the system were evaluated. The regeneration studies also showed that the uptake efficacy in the fifth cycle is reduced by 20% when compared with the first cycle. The results show that the biomass was a capable sorbent for the removal of CR9.