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Highly crystalline mesoporous anatase TiO2 nanospheres with high surface area (higher than P25 and anatase TiO2) are prepared by a soft-template method. Despite the high specific surface area, these samples have three times lower equilibrium adsorption (<2%) than Degussa P25. The rate constant of the mesoporous anatase TiO2 (0.024 min-1) reported here is 364% higher than that of P25 (0.0066 min-1), for the same catalytic loading. The results of oxidation-extraction photometry using several reactive oxygen species (ROS) scavengers indicated that mesoporous anatase TiO2 generates more ROS than P25 under UV-light irradiation. This significant improvement in the photocatalytic performance of mesoporous spherical TiO2 arises from the following synergistic effects in the reported sample: (i) high surface area; (ii) improved crystallinity; (iii) narrow pore wall thicknesses (ensuring the rapid migration of photogenerated carriers to the surface of the material); and (iv) greater ROS generation under UV-light. [ABSTRACT FROM AUTHOR]