A facile method to synthesize ZnO-TiO₂-layered double-nanostructures with the average thickness of 20 μm on a bamboo substrate was proposed to improve the antifungal and flame-retardant properties. The cross-linked wurtzite ZnO nanostructures with an average thickness of approximately 0.14 μm were uniformly distributed on the anatase TiO₂ surface. The energy-dispersive X-ray spectroscopy (EDS) confirmed that the ZnO-TiO₂ coating on bamboo was a layered double nanostructure. During a two-month antifungal test conducted in an outdoor environment, the fungi began to grow after one week on pristine bamboo and three weeks on ZnO-bamboo and TiO₂-bamboo. Furthermore, there was an infected area of 100% after four weeks for pristine bamboo and six weeks for ZnO-bamboo, while there was an infected area of 43% after eight weeks for TiO₂-bamboo. By comparison, there was no visible fungal growth on ZnO-TiO₂-bamboo until the end of the test. The electron spin resonance (ESR) technique has demonstrated that the reactive oxygen species (ROS) of •O₂⁻ and •OH were produced from the ZnO-TiO₂ surface under visible light irradiation (λ > 420 nm). This large quantity of •O₂⁻ compared to •OH is considered to be mainly responsible for the inactivation of fungi. Additionally, the limiting oxygen index has increased from 25.6% to 30.2% after being covered with a ZnO-TiO₂ coating, which revealed a significant enhancement of its flame-retardant property.