The escalating presence of dye pollutants in industrial effluents has rendered the pursuit of environmentally benign and economically sustainable remediation strategies increasingly imperative. Among emerging solutions, the application of biosorbents derived from agro-industrial residues, such as olive pomace, has garnered significant interest due to the low cost and promising efficiency of these residues. This study explores the sorption capabilities of biosorbents and biochars synthesized from olive pomane via water-activation and pyrolysis, respectively, for the removal of dye compounds from aqueous solutions. The materials underwent comprehensive characterization through BET surface area analysis, Raman Spectroscopy, Fourier transform infrared spectroscopy (FTIR), elemental analysis and scanning electron microscopy (SEM). Sorption performance was assessed using two representative dyes—Safranin and Methylene blue—while the kinetics, isotherms and pH influence on the sorption process were thoroughly investigated. Both dyes exhibited satisfactory removal rates, with no significant discrepancies observed in the sorption efficiency between the two, indicating the versatility of the material across different dye classes. The results revealed a markedly improved sorption capacity for the pyrolysed material relative to its water-activated counterpart, a performance attributed to its enhanced porosity and surface area. These findings underscore the potential use of biochar derived from olive pomace as an efficient, low-cost sorbent for dye-laden wastewater. Ultimately, this study highlights the valorization of agri-food by-products as viable tools for wastewater treatment, aligning with broader goals of circular economy advancement and sustainable waste management.