Sculptured thin films (STFs) are assemblies of nominally identical, parallel nanowires with tailored shapes such as chevrons and spirals. A series of iron(lll) STFs were produced with varied crystallinity (from hematite toferrihydrite) and nanowire shapes (slanted columnar, clockwise helical, and counterclockwise helical). When the dissimilatory metal-reducing bacterium Shewanella putrefaciens CN32 was used to measure their bioreducibility, it was found that bioreduction was controlled primarily by oxide crystallinity. STFs were characterized by scanning electron microscopy, atomic force microscopy, and grazing incidence small-angle X-ray scattering. Postbioreduction characterizations determined that mineralogy of the film materials did not change, but surface roughness generally increased. Changes caused by bioreduction were assessed in terms of both transmittance and reflectance of light incident normal to the STFs. The greatest optical changes were obtained with crystalline hematite films. These results underscore the feasibility of an STF-based fiber optic iron(lll) reduction sensor for in situ subsurface deployment.