In this letter, we present a simple one-step, versatile, scalable chemical vapor deposition (CVD)-based process for the encapsulation and stabilization of a host of single or multicomponent supramolecular assemblies (protcoliposomes, microbubbles, lipid bilayers, and photosynthetic antennae complexes and other biological materials) to form functional hybrid nanobiomaterials. In each case, it is possible (i) to form thin silica layers or gels controllably that enable the preservation of the supramolecular assembly over time and under adverse environmental conditions and (ii) to tune the structure of the silica gels so as to optimize solute accessibility while at the same time preserving functional dynamic properties of the encapsulated phospholipid assembly. The process allows precise temporal and spatial control of silica polymerization kinetics through the control of precursor delivery at room temperature and does not require or produce high concentrations of injurious chemicals that can compromise the function of biomolecular assemblies; it also does not require additives. This process differs from the conventional sol-gel process in that it does not involve the use of cosolvents (alcohols) and catalysts (acid or base).