Arsenic (As), a poisonous and carcinogenic heavy metal, affects human health and the environment. Numerous technologies can remove As from drinking water. Adsorption is the most appealing option for decentralized water treatment systems (DWTS) for small communities and household applications because it is reliable, affordable, and environmentally acceptable. Sustainable low-cost adsorbents make adsorption more appealing for DWTS to address some of the small communities’ water-related issues. This review contains in-depth information on the classification and toxicity of As species and different treatment options, including ion exchange, membrane technologies, coagulation-flocculation, oxidation, and adsorption, and their effectiveness under various process parameters. Specifically, different kinetic and isotherm models were compared for As adsorption. The characterization techniques that determine various adsorbents’ chemical and physical characteristics were investigated. This review discusses the parameters that impact adsorption, such as solution pH, temperature, initial As concentration, adsorbent dosage, and contact time. Finally, low-cost adsorbents application for the removal of As was discussed. Adsorption was found to be a suitable, cost-effective, and reliable technology for DWTS for small and isolated communities. New locally developed and low-cost adsorbents are promising and could support sustainable adsorption applications.