Arsenic (As) contamination of groundwater reservoirs is a global environmental and health issue given to its toxic and carcinogenic nature. Over 170 million people have been affected by As due to the ingestion of As-contaminated groundwater. Conventional methods such as reverse osmosis, ion exchange, and electrodialysis are commonly used for the remediation of As-contaminated water; however, the high cost and sludge production put limitations on their application to remove As from water. This review critically addresses the use of various agricultural waste materials (e.g., sugarcane bagasse, peels of various fruits, wheat straw) as biosorbents, thereby offering an eco-friendly and low-cost solution for the removal of As from contaminated water supplies. The effect of solution chemistry such as solution pH, cations, anions, organic ligands, and various other factors (e.g., temperature, contact time, sorbent dose) on As biosorption, and safe disposal methods for As-loaded biosorbents to reduce secondary As contamination are also discussed.