Volatile organic compounds (VOCs), recognized as hazardous air contaminants, prompt the exploration of sustainable air purification methods. Solar photocatalytic oxidation emerges as a promising solution, utilizing semiconductor photocatalysts like titanium dioxide (TiO2). However, the raw material crisis necessitates reduced TiO2 usage, leading to investigations into TiO2 modification techniques. The study introduces a novel approach by employing natural fibers, specifically loofah sponge, as a TiO2 support. This method aims to maintain photocatalytic activity while minimizing TiO2 content. The article explores using halloysite, a natural clay mineral, as a supportive material, enhancing mechanical strength and adsorption properties. The resulting TiO2/loofah‐halloysite composites are evaluated for their efficacy in gas‐phase photocatalytic oxidation of toluene and ethanol, chosen as representative VOCs. The conversion of toluene and ethanol on the composite was 88% and 39%, respectively, with high selectivity toward CO2. In addition to its high performance, the bio‐composite was stable for several conversion cycles, keeping the conversion activity unchanged. The study contributes to developing green hybrid materials for VOC removal, showcasing potential applications across industries.