A plasma polymerization method was employed to deposit an ultrathin pyrrole film of 3 nm onto the surfaces of single wall carbon nanotubes (SWCNTs) and Al2O3 nanoparticles for developing high-strength nanocomposites. The surfaces of plasma coated SWCNTs and Al2O3 nanoparticles were studied by high resolution transmission electron microscopy (TEM) and time-of-flight secondary ion mass spectroscopy. After sintering the SWCNTs-Al2O3 composites at different temperatures (maximum of 1200 °C), the thermal stability of plasma-coated SWCNTs was significantly increased, compared to their uncoated counterparts. After hot-press sintering, the SWCNTs without plasma coating were essentially decomposed into amorphous clusters in the composites, leading to degraded mechanical properties. However, under the same sintering conditions, the plasma surface modified SWCNTs were well preserved and distributed in the composite matrices. The effects of plasma surface coating on the thermal stability of SWCNTs and mechanical behavior of the nanocomposites are discussed.