The objective of this study was to find a suitable and versatile agroforestry waste as alternative low-cost biosorbents for the removal of inorganic and organic compounds present in the wastewater of tannery industry [leather dyes and Cr(VI)]. Grapefruit peelings, fern, eucalyptus barks, oak leaves and cane pruning of grapevines were evaluated as biosorbents. Among them, grapefruit peelings showed the best results reaching 45 and 55% for the mixture of dyes and Cr(VI), respectively. A significant improvement in the performance of this biosorbent was obtained when it was pretreated with H 2 O 2 (1 M) attaining the highest removal capacity of 80% and 100%, respectively. This biosorbent was characterised showing an adsorption capacity of 1.1003 meq/g and pH ZPC 3.48. The adsorption working parameters, kinetics and isotherms were deeply studied in order to scale up the process to a continuous treatment system. Adsorption isotherms data fitted well to the Langmuir model with a maximum uptake of 37.427 mg/g for dyes mixture and 39.0628 mg/g for Cr(VI). Finally, the dynamic behaviour of the system, operating at different flow rates, was evaluated using a Homogeneous Surface Diffusion Model. Pretreated grapefruit peelings demonstrated to be a suitable low-cost biosorbent in the treatment of wastewater of tannery industry.