Aluminosilicate mineral, imogolite, with chemical composition [(OH)(3)Al2O3SiOH] has high monodispersity of diameter originated by the arrangements of inner hydroxyl (OH) groups that induced the strain energy minimum due to hydrogen bond networks. We have successfully synthesized substituted imogolite with methyl groups (Me-imo) instead of inner hydroxyl groups. While imogolite prefers zigzag chirality, Me-imo prefers armchair chirality which was confirmed by the simulation and the x-ray diffraction (XRD) pattern. Me-imo has larger specific surface area and less hydrogen bond contribution than that of imogolite, which was confirmed by the Barrett-Joyner-Halenda (BJH) pore size distribution.