The present study aimed to investigate the adsorption capacity of two anionic dyes, namely, Congored (CR) and Coralene Dark Red2B (DR), onto prepared alginate (Alg) and chitosan(Cs) biopolymer films. The two biopolymers were combined at different mass ratios using a “solvent-cast” process to incorporate their unique properties and evaluate their effectiveness in removing the dyes. All samples were characterized by means of Fourier transform infrared spectroscopy (FTIR), differential scanning calorimetry (DSC), scanning electron microscopy (SEM) and determination of point of zero charge (pH_pzc). The swelling ratios were determined by gravimetric measurements. The effects of pH, adsorption time, thickness, temperature and initial concentration of CR and DR dyes on the adsorption results were studied systematically. The dye adsorption kinetics showed that the Alg/Cs films at % proportions of 75/25, 50/50, 25/75 and 0/100 reached equilibrium from 30 min to 180 min with high removal efficiencies that varied between 222.30 mg/g and 842.36 mg/g. The adsorption mechanism of CR and DR onto the synthesized biofilms was confirmed through Langmuir isotherm and the kinetics fitted well by the pseudo-second-order model, suggesting a monolayer and chemisorption process. The thermodynamic results demonstrated the spontaneity and the feasibility of the process as well as the exothermic nature. Hence, the findings revealed that the Alg/Cs biofilms could be employed as potential natural adsorbents for the removal of anionic dye pollutants from aqueous environments.