MWNTs of various sizes were compounded into SPI matrix by solution mixing and then compression-molded into nanocomposite sheets, which were characterized by XRD, SEM, TEM, and tensile and water uptake testing. The resultant nanocomposites showed improved mechanical performance and higher water resistance depending on MWNT size and content. This work details a strategy to achieve improved performance, especially in terms of mechanical properties, using MWNTs of various sizes to regulate the entanglement and penetration between SPI and MWNTs.