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In 1991, Bickley et al. proposed a synergetic effect between anatase and rutile in Degussa P25. Since then, there has been an intensive debate about the correctness of this proposal, the origin of the synergism, and the right polymorph composition. However, a comparison of pure titanium dioxide samples with various anatase-to-rutile ratios, but otherwise identical properties, is missing. In this paper, we report about a series of utterly pure, highly porous titanium dioxide films with identical grain sizes, surface areas, and crystallinity, but varying polymorph compositions. Photocatalytic oxidation of methylene blue was utilized to investigate the influence of the anatase-to-rutile ratio on the photoreactivity. We clearly observe the synergetic effect within a well-defined range of anatase-to-rutile ratios. A film with ∼60% anatase and ∼40% rutile exhibits optimal performance at a 50% improved activity compared with pure …