We investigate the electronic coupling between a TiO2 nanowire and a natural dye sensitizer, using state-of-the-art time-dependent first-principles calculations. The model dye molecule, cyanidin, is deprotonated into the quinonoidal form upon adsorption on the wire surface. This results in its highest occupied molecular orbital (HOMO) being located in the middle of the TiO2 bandgap and its lowest unoccupied molecular orbital (LUMO) being close to the TiO2 conduction band minimum (CBM), leading to greatly enhanced visible light absorption with two prominent peaks at 480 and 650 nm. We find that excited electrons are injected into the TiO2 conduction band within a time scale of 50 fs with negligible electron-hole recombination and energy dissipation, even though the dye LUMO is located 0.1-0.3 eV lower than the CBM of the TiO2 nanowire.