The work pursued aids art historians in a better understanding of the diverse techniques of illumination and writing and conservators and restorers to better orient their methods of treatment. A part of this report summarizes the completed work in the identification of components which have been utilized in the production of black ink of ancient manuscripts while the other part is exclusively dedicated to pigments and their utilization in the pictorial layers of illuminations of Serbian manuscripts. Various techniques of identification were utilized; microscopy, microchemical analysis, infrared spectrophotometry, cross sections, gas phase chromatography, and x-ray fluorescence.