This study demonstrates the efficient removal of Alizarin Yellow R anionic dye (AY) from aqueous solutions using green adsorbents. Natural kaolin clay (A1), acid-modified natural clay (A2), chemically treated orange peel (C1) and biochar produced by the thermal treatment of orange peel (C2) were tested for the adsorption of AY. The characteristics of the sorbents were determined by instrumental methods: SEM, EDS, FTIR, BET and TGA. The adsorption experiments were performed under different conditions, including the initial AY dye concentration, adsorbent weight, pH, temperature and contact time. The maximum adsorption capacities had values between 15.72 and 74.62 mg/g at 298 K and the optimal pH of 6.5 at initial concentrations ranging from 30 to 70 mg/L for all adsorbents. The equilibrium data were used for the adsorption isotherm models: Freundlich, Langmuir and Temkin. The Freundlich model fit best for the adsorbents A2, C1 and C2, and the Langmuir isotherm had the highest regression value for the adsorbent A1 (R2 = 0.9935). Thermodynamic parameters indicated the spontaneous and favorable adsorption process of AY. A study of the adsorption kinetics proved that they best fit the pseudo-second-order model, with the highest coefficients of determination (R2), outperforming the pseudo-first-order model. The results of this study indicate the potential for the valorization of locally available clays and orange peel waste in the purification processes of water.