Metal-organic semiconductor films are fabricated as co-evaporated films. It is demonstrated that the technique can be used to fabricate metal-semiconductor surface-enhanced Raman scattering (SERS) or surface-enhanced resonance Raman scattering (SERRS) substrates or to attain SERS or SERRS of highly insoluble pigments. The experiments are carried out using three different pigments: iron phthalocyanine (Fe Pc) and two substituted tetracaboxylic perylenes (PTCDs). The structure of the co-PVD films was characterized at the nanoscale by scanning electron microscopy through field-emission gun (SEM-FEG), revealing a fairly homogeneous spatial distribution of the silver-pigment nanoparticles. The fabricated mixed nanostructures show a homogenous distribution of plasmon enhancement as observed in the point-by-point mapping of the SERRS spectra recorded with micrometer spatial resolution in Raman microscopy.Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP)Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)