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In this study, we completed a simple low-temperature synthesis of nest-like titanium oxide (TiO2) microspheres with exposed (001) facets. For the first time, the photocatalytic performance was enhanced by sodium hydroxide (NaOH) alkalization. The characterization of as-synthesized F-TiO2 and OH-TiO2 were analyzed by field emission scanning electron microscopy, high-resolution transmission electron microscopy, X-ray diffraction, fourier transform infrared spectroscopic analysis, ultraviolet-vis diffuse reflection spectra and Raman spectroscopy. The photocatalytic activity of the as-prepared catalyst was evaluated through the photocatalytic degradation of methylene blue (MB) and Rhodamine B (RhB) under simulated solar light. The results showed that modification using NaOH can lead to an increase in the percentage of (001) facets from 27.8% for F-TiO2 to 39.2% for OH-TiO2. OH-TiO2 showed superior catalytic photoactivity toward MB. The mechanism of NaOH on TiO2 is also discussed.