Vermiculite and fluor-tetrasilicic mica were intercalated with alkali metals (Na, K and Rb) by vapor transport. X-ray and Raman scattering experiments were conducted to study the structure and lattice dynamics of the new clay compounds. When Rb and K atoms were intercalated to the host materials, superlattices were formed. In Na intercalated compounds, however, no superlattice x-ray diffraction peaks were found. Raman spectra exhibited drastic changes after alkali-metal intercalation, reflecting the structural changes found bf our x-ray diffraction.