A novel self-assembly strategy of ordered silica arrays on halloysite clay nanotubes allows us to obtain mesoporous MCM-41 materials with enhanced thermal and mechanical stability. The formation of a structured mesoporous silica phase on halloysite is based on the assembly of cationic amphiphilic molecules onto a negative nanotube surface. The resulting MCM-41/halloysite composite demonstrated thermal and mechanical stability up to 1100 °C and 500 MPa showing great potential for application of mesoporous materials as industrial catalyst carriers and adsorbents.