Arsenic contamination of drinking water and groundwater remains a major global public health and environmental concern because of the high toxicity of inorganic Arsenic species and their widespread occurrence from both natural and anthropogenic sources. Conventional physicochemical treatment methods often face limitations of high cost, secondary waste generation, incomplete removal of arsenite, and operational complexity. Hybrid systems that combine bioremediation with nanostructured materials provide synergistic advantages by integrating the high surface area, reactivity, and separability of nanomaterials with the cost-effectiveness, selectivity, and biotransformation potential of microorganisms or biosorbents. This review synthesises recent advances in hybrid technologies for the removal of aqueous Arsenic. Four representative categories are examined: live-cell magnetic nanoparticle systems, graphene oxide–iron nanohybrids integrated with microbial activity, biochar-supported magnetic nanocomposites, and nZVI-influenced microbial or bio-nanocomposite systems. Hybrid approaches consistently show higher adsorption capacities, faster kinetics, improved stability, and easier recovery than standalone biological or nanostructured methods. Remaining challenges include long-term performance in complex real-water matrices, potential nanomaterial ecotoxicity, regeneration efficiency, and scale-up. Future research should prioritise green synthesis, multifunctional materials capable of simultaneous oxidation and adsorption, pilot-scale validation, and life-cycle assessment to support sustainable implementation.