Radially layered copolymeric poly(amidoamine-organosilicon) (PAMAMOS) dendrimers have been prepared with hydrophilic polyamidoamine (PAMAM) interiors and hydrophobic organosilicon (OS) exteriors. At low degrees of surface derivitization with trimethylsilyl groups these dendrimers significantly reduce water surface tension. At higher degrees they become insoluble and form spread monolayers on water which on compression can sustain surface pressures of over 50 mN/m due to the strong attraction of the PAMAM core to the water surface. When reactive organosilicon terminating units such as methoxysilyl-groups are incorporated, the copolydendrimers can be crosslinked into networks. These new elastomeric or plastomeric dendritic materials have well-defined, nanoscopic domains with the ability to complex and encapsulate within the PAMAM domains, a wide variety of metal compounds and metal atoms.