Ghana’s artisanal and small-scale mining (ASM) releases harmful contaminants, including arsenic, into the environment at levels exceeding acceptable limits. For miners to reduce arsenic levels in their tailings before discharge, the cost of remediation materials and processes must be significantly lower than it is now. This study uses unactivated and activated chars produced from agricultural waste, informed by the United Nations Food and Agriculture Organization and other studies on traditional charcoal-making methods, to assess the potential of sorption techniques to reduce arsenic levels in tailings, both alone and when combined with iron oxide-coated sand (IOCS). Sorption phenomena were measured through batch and column experiments. The Freundlich and Langmuir sorption isotherms were used to characterise the adsorbents. IOCS alone achieved an average removal efficiency of 91.65%, compared with 40.20%, 37.40%, and 21.40% for the unactivated chars, and 76.83%, 73.5%, and 78.83% for the activated chars from sawdust, coconut husk, and neem wood feedstocks, respectively. The column experiment combining IOCS and activated chars in a multi-layer, four-stage system achieved 100% removal efficiency within 46 hours. Generally, the traditional charcoal preparation method can be used to produce effective, low-cost adsorbents from agricultural waste for arsenic removal from mining effluents. Employing a combination of activated chars and IOCS results in rapid arsenic removal. A consistent approach to prevent the ASM industry from contaminating Ghana’s water resources with excessive arsenic is to issue directives requiring the use of activated chars made from agricultural waste, combined with IOCS for mine remediation. This strategy can also generate multiple alternative employment opportunities within the mining sector.