Vanadium phosphorus oxide (VPO) has been embedded in a titania matrix. The adsorption capacity of the VPO(5-30 wt %)@TiO2 composites and VPO alone for the removal of harmful cationic and anionic dyes such as methylene blue (MB), rhodamine B (RhB), and methyl orange (MO) have been extensively investigated. The FT-IR, XRD, TGA, FE-SEM, EDX, and BET techniques were applied for characterization of the adsorbents. Batch-adsorption experiments demonstrated that the VPO(30 wt %)@TiO2 as the best composite selectively removes MB with more than 94% removal efficiency. The adsorption behavior of the MB on the VPO(5-30 wt %)@TiO2 composites was investigated with variations in the mass of sorbent, initial dye concentration, solution pH, temperature, and contact time. Kinetic experiments demonstrated that the pseudo-second order kinetic model showed the best fit with the adsorption data. The efficiency of the VPO(30 wt %)@TiO2 as the preferred composite remained unchanged after five adsorption cycles, and could be regenerated easily by simple washing with NaOH (0.1 mol/L) and water.