Arsenic (As) is the world's most hazardous chemical found in drinking water of many countries, thus there is an urgent need for the development of low-cost adsorbents for its removal. Here we report a highly versatile and synthetic route for the preparation of a three dimensional (3D) graphene-iron oxide nanoparticle aerogel composite for the efficient removal of As from contaminated water. This unique 3D interconnected network was prepared from natural graphite rocks with a simple reaction without the use of harsh chemicals, which combines the exfoliation of graphene oxide (GO) sheets by the reduction of ferrous ion to form a graphene aerogel composite decorated with iron oxide nanoparticles. The prepared adsorbent showed outstanding absorption performance for the removal of As from contaminated water, due to its high surface-to-volume ratio and characteristic pore network in the 3D architecture. The performed case study using real drinking water contaminated with As under batch conditions showed successful removal of arsenic to the concentration recommended by the World Health Organization (WHO).