The synthesis and characterization of a series of organosilicon sheet polymers from the natural occurring mineral apophyllite, KCa₄Si₈O₂₀(F,OH)∙8H₂O, has been carried out. In this series the pendent siloxy groups grafted to the silicate backbone were R(CH₃)₂SiO (R = 1,4,6,10 or 18 carbon chain, or R = functionalized propyl groups such as chloropropyl or cyanopropyl). The intersheet spacings were determined by X-ray powder diffraction and were found to correlate with the pendent group chain length. Multiple pendent group polymers were also synthesized, where a pendent group with a short polar chain, such as (NCC₃H₆)(CH₃)₂SiO, was grafted to the backbone in conjunction with a long carbon chain containing pendent group. One example of such a polymers is [((C₁₈H₃₇)(CH₃)₂SiO)_x((NCC₃H₆)(CH₃)₂SiO)_y(OH)_1-x-ySiO_1.5]_n, A--ODM₂-CM₂. These sheet polymers have been found to form gels with both polar and non-polar solvents; the sheets in these gels are well separated (as characterized by X-ray powder diffraction). Organosilicon sheet polymers with functional groups, such as a hexenyl group, have also been synthesized. Sheet polymers with a combination of functional and polar pendent groups offer promise in the creation of organosilicon polymer nanocomposites.

The multiple functional groups on the silicate backbone create a system in which the silicate layers can be easily exfoliated in non-polar fluids and also allow for further reactivity including hydrosilylation. The sheet polymer A--HEM₂-CM₂, [((C₆H₁₃)(CH₃)₂SiO)_x((NCC₃H₆)(CH₃)₂SiO)_y(OH)_1-x-ySiO_1.5]_n, was synthesized and was processed by gelling it with an organic solvent followed with lyophylization of the gel. The processed A--HEM₂-CM₂ was mixed with a functionalized siloxane and sonicated. This method avoided mechanical mixing and gave nanocomposite monoliths in which the silicate filler was very well dispersed.