A series of aluminum-containing kanemite (Al–kanemite) samples with several Si/Al molar ratios were synthesized. The Al–kanemite samples were pillared with silica. X-ray diffractograms showed that the layered structure of the Al–kanemite samples was maintained at Si/Al=∞∼10 but was broken at Si/Al = 5, 2.5, and 1. 29 Si MAS NMR spectra of the Al–kanemite samples, except for that of Si/Al = 1, mainly showed peaks of Q 3 sites, which were attributed to Si(OSi) 3 (OH) groups, although peaks assigned to Si(OAl)(OSi) 2 (OH) were also seen. The 27 Al MAS NMR spectra indicated that the Al–kanemite samples had only four-coordinate aluminum atoms. The FTIR spectra of pyridine adsorbed on the pillared Al–kanemite derivatives revealed Lewis acid sites on the surface. The nitrogen adsorption isotherms of the derivatives were classified as type I (Langmuir) absorption isotherms. Using the α s method, the specific surface areas of the derivatives were 572–756 m 2 g −1 , and the pore sizes were calculated as 1.25–1.83 nm. The pillared Al–kanemite derivatives had slit-shaped micropore structures.