Novel and low cost chemically modified masau stone (CMMS) was investigated for its biosorption of an anionic azo dye, Orange II (OII), and toxic hexavalent chromium (Cr(VI)) from aqueous systems: individually, simultaneously and consecutively. XPS and FTIR analyses indicated the introduction of quaternary-Nitrogen to the CMMS surface after activation with epichlorohydrin (etherifying agent) and diethylenetriamine (crosslinking agent). The effects of pH, contact time and initial concentration (C), and loading order on mechanisms of biosorption/reduction of OII and Cr(VI) onto CMMS were examined in detail. Several analytical techniques were employed to characterise the physio-chemical properties of the CMMS and determine the biosorption mechanisms. The pseudo second order and redox models were able to adequately predict the kinetics of biosorption. The Langmuir maximum OII biosorption capacity (q) was calculated as 136.8 mg/g for the dye onto the Cr(VI)-loaded CMMS consecutive system at C = 100 mg/dm. The q for the Cr(VI) system was found to be 87.32 mg/g at the same C max. This reveals that the biosorption of OII and Cr(VI) mainly takes place via two different mechanisms i.e. hydrogen bonding and electrostatic attraction for the dye, and biosorption-coupled reduction for Cr(VI).