BACKGROUND: Simultaneous removal of arsenic and fluoride anions from water by adsorption remains a challenge for environmental remediation practice. To address this issue, four mesoporous bimetallic oxides (MBOs) were prepared via the evaporation-induced self-assembly (EISA) method and studied as adsorbents for the co-uptake of arsenate (As(V)) and fluoride (F − ) from synthetic wastewater. Adsorption envelope and equilibrium experiments were performed to investigate the adsorption behaviors and properties.RESULTS: These composites possessed high surface areas (e.g. 200 m 2 g −1 for meso-Ti/Al) and well-defined mesopores, enabling high adsorption capacities for both As(V) and F − . The maximum adsorption capacities of mesoporous titanium-lanthanum oxide (meso-Ti/La) were as high as 81.42 mg g −1 and 44.37 mg g −1 for As(V) and F − , respectively. Surface complexation modeling indicates that As(V) removal mainly involved bidentate surface complexation with surface ≡Me-OH, while F − was retained by formation of monodentate surface complexes. CONCLUSION: The removal mechanisms were confirmed by X-ray photoelectron spectroscopy. These MBOs were found to be effective for simultaneous removal of arsenic and fluoride from water. This study also demonstrated that the incorporation of multi-components and mesoporosity into one composite is an efficient strategy for design and application of high-efficiency adsorbents for environmental remediation of aqueous contaminants.