To examine how London energy controls the c-dimensions of phyllosilicates, London energy, as well as Coulomb and Pauli repulstion energy was calculated as a function of d(001) for 1M and d(002) for 2M 1 phyllosilicates. London and Pauli repulstion energy calcualtion use a direct interaction calculation method and Coulomb energy calculation adopts Fourier synthesis method. The energy calculations show that Coulmb and Pauli repulsion energy dominantly control the c-dimensions of phyllosilicates having the interlayer cationss, i.e., the layer charges. On the other hand, if phyllosilicates have no interlayer cations, London energy is solely responsible for holding the layers and maintain the c-dimensions. The significance of London energy in determining the c-dimensions of phyllosislicates de-creases as the layer charge increases. When the layer charge is lower than one equivalent on the basis of Oη(OH)2 formula, London energy plays an important role in determing the c-dimensions. however, if the layer charge is higher than one equivalent, London energy becomes insignifi-cant in determining the c-dimension.