Imperfect oriented attachment of nanoparticles over specific surfaces is rationalized to cause accretion and defects for the hexagonal inorganic-surfactant mesophase. Analytical electron microscopy indicates that silicate MCM-41 particles, prepared in alkaline hydrothermal condition and then surfactant (cetyltrimethylammonium bromide) leached, have well-developed {10} surfaces with monolayer steps and a rather uniform base with constant tubular wall thickness. These surfaces are beneficial to {10} vicinal and head-on attachment, causing respectively edge dislocation and twist boundary for hexagonal silicatropic liquid crystal. Brownian motion may proceed above a critical temperature for anchorage release at the interface of imperfectly attached particles until an epitaxial relationship is reached.