A method to control the number of layers of dispersed silicate platelets was investigated. In order to achieve control over the number of layers, a layered silicate with two antagonistic properties, swelling and nonswelling, was prepared in each particle. A new regularly interstratified layer silicate composed of talc/talc/smectite (TTS) in an ordered sequence was synthesized using a hydrothermal technique. A novel layered silicate‐polymer nanocomposite was then prepared through exfoliation of the regularly interstratified TTS. The controlled morphology of the nanocomposite indicates that silicate nanolayers consisting of three layers/group are uniformly dispersed in the polymer matrix, which suggests a method for the control of the number of dispersed layers in polymer nanocomposite technology. More importantly, this new composite system could extend the field of high‐performance materials beyond traditional applications to encompass new unexpected functionality.