Unique low-dimensional SiO(2)-based nanomaterials can be encapsulated and synthesized inside the nanometer-scale one-dimensional internal spaces of carbon nanotubes (CNTs). In this study, various single-walled CNTs (SWNTs) and double-walled CNTs (DWNTs) having different diameters are used as containers for cubic octameric H(8)Si(8)O(12) molecules. High-resolution transmission electron microscopy (HRTEM), Fourier transform infrared (FT-IR) spectroscopy, and Raman spectroscopy observations revealed that, depending on the diameter of the CNTs, two types of structures are formed inside the SWNTs and DWNTs: In the case of those CNTs having inner diameters ranging from 1.2 to 1.4 nm, a new ordered self-assembled structure composed of H(8)Si(4n)O(8n-4) molecules was formed through the transformation of H(8)Si(8)O(12); however, in the case of CNTs having inner diameters larger than 1.7 nm, a disordered structure was formed. This behavior may indicate that strong interactions occur between the CNTs and the encapsulated H(8)Si(4n)O(8n-4) molecules.