Naturally occurring tubular iron oxides produced by aquatic bacteria in Leptothrix spp. are promising raw materials for hematite-based red pigments because of the higher heat resistance as compared with chemically synthesized hematite compounds. Here, we report iron oxide red pigments prepared through an additive deposition of aluminum on culture-based biogenous iron oxide (cBIOX) sheaths using an artificial culture system of L. cholodnii strain OUMS1. The heat-treated Al-containing cBIOXs exhibited elevated chroma and lightness along with increasing Al contents and enhanced thermal stability of color tones to repetitive heat treatments. XRD analysis showed a monophasic pattern of hematite in the Al-rich cBIOX after heating at a wide range of high temperatures. Micromorphology analyses revealed that putative Al oxide regions present among hematite particles plausibly prevented the grain growth of hematite during heat treatments. The results therefore demonstrate that the bioderived Al-rich iron oxide sheaths can serve as innovative inorganic red pigments feasible for industrial applications.