The wide bandgap semiconductor TiO2 has become the dominant UV-activated photocatalyst in the field of air and water detoxification because of its high stability, low cost, high oxidation potential and chemically favorable properties. The demand for visible-light activated photocatalytic systems is increasing rapidly; however, currently, the efficiency and availability of photocatalysts that can be activated effectively by the solar spectrum and particularly indoor lighting is severely limited. In this paper, a new coprecipitation/hydrolysis synthesis route is used to create a TiO2-ZnFe2O4 nanocomposite that is directed towards extending the photoresponse of TiO2 from UV to visible wavelengths (>400nm). The effect of TiO2's accelerated anatase-rutile phase transformation due to the presence of the coupled ZnFe2O4 narrow bandgap semiconductor is evaluated. The transformation's dependence on pH, calcination temperature, particle size, and ZnFe2O4 concentration has been analyzed using XRD, SEM, and UV-Visible spectrometry. The requirements for retaining the highly photoactive anatase phase present in a ZnFe2O4 nanocomposite are outlined. The visible-light activated photocatalytic activity of the TiO2-ZnFe2O4 nanocomposites have been compared to an Aldrich TiO2 reference catalyst, using a solar-simulated photoreactor for the degradation of phenol.