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Abstract: We describe recent progress in the imprinting of bulk silica employing both covalent and non-covalent approaches and over multiple length scales spanning 1-15 nm. In the covalent approach, thermolysis is used as a driving force for imprint fragment removal for the imprinting of amines and thiols in bulk silica. This is accomplished using small molecules as templates for achieving organization on the length scale of about 1 nm. In the non-covalent approach, we report on the use of gold nanoparticles as templates for imprinted silica synthesis, with a diameter of approximately 15 nm. We summarize previous approaches for the synthesis of imprints derived from gold-silica core-shell nanoparticles, involving the self-assembly of aminosilane on colloidal gold surfaces. Finally, we describe our efforts to use the strong interaction between thiols and gold for the imprinting of several thousand thiolates within silica pores commensurate in size to the nanoparticle templates used.