Photoinduced electron-transfer (ET) dynamics in Fe(II)(CN)64- sensitized TiO2 nanoparticles in D2O solution are studied by subpicosecond tunable laser spectroscopy in the mid-infrared and visible region. The dynamics of the injected electrons are monitored by the mid-IR absorption of electrons in the semiconductor, and the corresponding dynamics of the adsorbate are monitored by the vibrational spectra of the CN stretching mode region and electronic absorption in the visible. After 400 nm excitation, the forward electron injection time from Fe(II)(CN)64- to TiO2 occurs in 1 ns (35%). Combining with previous measurements in the nanosecond to microsecond time scale (Lu et al. J. Am. Chem. Soc. 1993, 115, 4927 and Vrachnou et al...