The study of the support of three magnificent Armenian manuscripts produced in the 17th century was driven because the possibility of paper support was considered. The Bible LA 152 and the Gospels LA 193 and LA 253 were made in the Armenian diaspora, in Crimea and Constantinople, respectively. Micro‑Fourier transform infrared spectroscopy and micro-ATR spectroscopic imaging proved that collagen was present with variable amounts of calcium carbonate in the Bible LA 152, Gospels LA 193, and LA 253. Furthermore, calcium carbonate is dominant in the Bible LA 152. Other compounds were also identified. In the Bible LA 152, a Si-O-based compound, and in Gospel LA 253, a cellulose-based material. The Si-O-based compound was detected both by ATR and transmission. It can be a glass compound applied as a powder, which needs to be further explored. The C-H region is highly relevant, as it opens up the possibility of using a tempera based on egg white for the two Gospels. This practical application of the research findings could have significant implications for future manuscript studies, underscoring the importance of this research and its potential to influence the practical aspects of manuscript production.