Contamination of water by chromium (Cr) creates serious pollution in terms of the environment and public health, since its different forms become released into air, water, soil and residential areas. In the present work, olive leaf powder (OLP) was evaluated as a novel low-cost sorbent due to its various functional groups such as amide, hydroxyl, carboxyl, and carbonyl which are responsible for the bio-removal of chromium ions from aqueous solutions. The chemical functional groups and microstructure of the OLP bio-sorbent were characterized by the Fourier Transform Infrared (FT-IR) spectroscopy and scanning electron microscopy (SEM) techniques. The bio-sorption conditions were optimized as pH 4, contact time 60 min, bio-sorbent dosage 40 g/L, temperature 40 °C. The bio-sorption isotherm was well fitted to the Langmuir model, and the predicted maximum bioremoval capacity of the OLP was estimated at 42.4 mg/g under the above-mentioned experimental conditions. The reuse performance of the bio-sorbent was determined after repeated sorption/desorption cycles. The thermodynamic examination showed that the chromium sorption by OLP was endothermic in thermal nature. The kinetic evaluations indicated that the bio-sorption process well followed with the pseudo-second-order model. The overall results demonstrated that the OLP can be thought as a potential bio-sorbent for cleaning of chromium-contaminated water and wastewater due to its advantageous properties such as low cost, availability, renewable nature, and remarkable bio-sorption capacity.