The Ti-incorporated metal–organic framework structure, MIL-125, its amine-functionalized form, MIL-NH₂ and its surfactant-assisted version, SMIL-NH₂ were synthesized via a solvothermal route. The samples were characterized by XRD, SEM, EDS, UV-vis spectroscopy, and N₂ adsorption–desorption measurements. In the presence of a nonionic surfactant, cylindrical SMIL-NH₂, with 50–250 nm particle size, was obtained. The photocatalytic properties of the materials were evaluated by deoximation reaction. Compared with MIL-NH₂, the nanostructured SMIL-NH₂ MOF has more than double the surface area and is able to catalyze the regeneration of carbonyl compounds from various oximes at twice the rate in an energy-efficient photocatalytic system. Furthermore, it has been successfully shown that this new nanostructured photocatalyst is significantly durable under the reaction conditions and can be easily recycled after the reaction, with significant retention of its photocatalytic activity.