Ti-containing species are grown-on-tip ZnO nanopyramids for surface functionalization. This yields a remarkable enhancement of photoactivated superhydrophilic behavior, self-cleaning ability, and photocatalytic performances in comparison to bare ZnO. The reasons accounting for such an improvement are unravelled by a multitechnique analysis, elucidating the interplay between material chemico-physical properties and the corresponding functional behavior (ACS Applied Materials & Interfaces 11, 2019, 15881).