It has become one of the major environmental problems for people worldwide to be exposed to high arsenic concentrations through contaminated drinking water, and even the long-term intake of small doses of arsenic has a carcinogenic effect. As an efficient and economic approach for the purification of arsenic-containing water, the adsorbents in adsorption processes have been widely studied. Among a variety of adsorbents reported, the metal oxide heterostructures with high surface area and specific affinity for arsenic adsorption from aqueous systems have demonstrated a promising performance in practical applications. This review paper aims to summarize briefly the metal oxide heterostructures in arsenic removal from contaminated water, so as to provide efficient, economic, and robust solutions for water purification.