Hybrid organic-inorganic thin films exhibiting patterned structuring on the nanometer scale have been prepared through the
controlled hydrolysis-condensation of enantiomerically pure chiral urea-based silyl compounds. The thin films are obtained by
spin-coating of sols obtained via acid- or base-catalyzed hydrolytic condensation of these molecular precursors. A self-templating
process is demonstrated via atomic force and transmission electron microscopy, showing the formation of nanometer size
aggregates consisting of interconnected spherulates under acidic condition and of assembled fibers under basic conditions.