Organic arsenic acids (OAAs) are regarded as water pollutants because of their toxicity and considerable solubility in water. Adsorption of OAAs such as phenylarsonic acid (PAA) and p-arsanilic acid (ASA) from water was investigated over functionalized (with OH groups) metal-organic framework (MOF, MIL-101), as well as over pristine MIL-101 and commercial activated carbon. The highly porous MIL-101 bearing three hydroxyl groups (MIL-101(OH)3) exhibited remarkable PAA and ASA adsorption capacities. Based on the effects of pH on PAA and ASA adsorption, hydrogen bonding was suggested as a plausible mechanism of OAA adsorption. Importantly, OAAs and MIL-101(OH)3 can be viewed as hydrogen-bond acceptors and donors, respectively. Moreover, MIL-101(OH)3 could be regenerated by acidic ethanol treatment, being a promising adsorbent for the removal of PAA and ASA from water.