Diatom-templated noble metal (Ag, Pt, Au) and semiconductor (CdTe) nanoparticle arrays were synthesized by the attachment of prefabricated nanoparticles of defined size. Two different attachment techniques-layer-by-layer deposition and covalent linking-could successfully be applied. The synthesized arrays were shown to be useful for surface-enhanced Raman spectroscopy (SERS) of components, for catalysis, and for improved image quality in scanning electron microscopy (SEM). Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.