This article presents a preparation method for modified bamboo and explores its potential application as filler material in cooling towers. The study employs a dual-nanoparticle synergistic modification approach combined with silane-based interfacial optimization, utilizing nano-aluminum oxide and silicon dioxide modifiers to enhance the properties of bamboo. Molecular dynamics simulations reveal the reaction mechanisms between the silane coupling agent and the surfaces of the nanoparticles, which significantly improve the interfacial bonding between the bamboo and the modifiers. Scanning electron microscopy and thermal performance tests show that the modified bamboo exhibits notable improvements in thermal conductivity, thermal diffusivity, and specific heat capacity. These enhancements are attributed to the incorporation of aluminum oxide and silicon dioxide, which effectively boost the bamboo’s thermal conductivity and stability. Additionally, the surface hydrophilicity of the modified bamboo increases, resulting in a reduced contact angle and stronger hydration behavior. The modified bamboo can serve as a sustainable alternative to polyvinyl chloride fillers, reducing environmental impact and promoting resource sustainability. The bamboo modification strategy proposed in this work not only improves thermal transport properties but also offers a viable solution for replacing conventional polyvinyl chloride filler materials, delivering significant environmental and economic benefits.