Three different morphologies of FeTiOx materials (microcubes, etched-microcubes and microspheres) were prepared by a facile method using acid leachate of ilmenite as the precursor. The three FeTiOx materials exhibited different adsorption performance for Congo red (CR). Among them, the FeTiOx microspheres showed the highest adsorption capacity (723.8 mg/g) for CR, followed by the FeTiOx etched-microcubes (617.8 mg/g) and the FeTiOx microcubes (296.5 mg/g). Characterization results showed that the three FeTiOx materials had distinctive phase composition, pore structure and surface functional group, which ultimately lead to their difference in adsorption performance. The adsorption mechanism of the three FeTiOx materials mainly includes ion exchange, electrostatic adsorption and mesopore filling, but the contribution of each type is different.