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• Materials and Methods
• Fig. S1. Photographs of the mixed solution for the preparation of the mesoporous TiO₂ microspheres during the evaporation of the solvent THF.
• Fig. S2. TEM images with different magnifications of the sample taken from the preparation solution after the solvent evaporation at 40°C for 6 hours.
• Fig. S3. STEM image and EDX elemental maps of the sample taken from the preparation solution after THF evaporation at 40°C for 6 hours.
• Fig. S4. WAXRD patterns of the precipitates obtained at different solvent evaporation times without calcination.
• Fig. S5. The proposed mechanism for oriented growth of the anatase single-crystal–like pore walls.
• Fig. S6. HAADF-STEM images of a single ultramicrotomed 3D open radially oriented mesoporous TiO₂ microspheres.
• Fig. S7. SEM images of the products obtained after the second-step evaporation at a high temperature of 120°C.
• Fig. S8. TEM images of an ultramicrotomed radially oriented mesoporous TiO₂ microsphere with different integrity.
• Fig. S9. SAED and HRTEM images taken from the cylindrical pore bundle regions with different orientation.
• Fig. S10. HRTEM and SEAD images of the mesoporous TiO₂ spheres taken from the area of the cylindrical pore bundles.
• Fig. S11. Detail photovoltaic parameters of 15 individual mesoporous TiO₂ microsphere-based cells.
• Fig. S12. Independent certificate by the National Center of Supervision and Inspection on Solar Photovoltaic Products Quality.
• Fig. S13. Cross-sectional and top-view SEM images of the photoanode film based on the uniform mesoporous TiO₂ microspheres.
• Fig. S14. Photocatalytic decomposition of methylene blue dye over the mesoporous TiO₂ microspheres.
• Fig. S15. Cryo-SEM images of the samples harvested at different intervals of solvent evaporation time.
• Fig. S16. STEM image and EDX elemental maps of a single ultramicrotomed mesoporous TiO₂ microsphere.
• Fig. S17. SEM images of the products obtained under similar conditions in the absence of Pluronic F127.
• Fig. S18. Field-emission SEM (FESEM) and TEM images of the ordered mesoporous TiO₂ bulks with randomly oriented cylindrical pores.
• Fig. S19. HRTEM images, nitrogen adsorption-desorption isotherms, pore size distributions, and SAXS integral curves of the randomly oriented mesoporous TiO₂ bulk samples.

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