This work presents the study of an XIII century French medieval Legendarium manuscript. The manuscript has a complex background of destruction and restoration attempts. Now the manuscript consists of 214 sheets encapsulated in polyethylene terephthalate conservation envelopes. The damaged manuscript sheets are in different states, some illustrations and text sections are in rather bad condition, some pages contain blurred traces of pigments and inks, which were used to write letters and make illustrations. Works carried out on this unique literary monument, included research using optical microscopy (OM), infrared reflectography (IRR), micro-Raman spectroscopy, and Scanning Electron Microscopy (SEM). The work was aimed at the estimation of the manuscript preservation and its current state. It has been demonstrated that even the study of micro-particles can be useful in the initial stages of the parchment manuscripts study that are in highly damaged condition. A wide variety of materials, which were used in different periods of time, have been found. Two types of red and four types of blue pigments were found in the studied particles from parchment. Locating the particles of iron-gall ink and pigments (for example, cinnabar and azurite) in the same region may indicate a possible use of this type of ink for both text and decoration. Pigments were revealed, the appearance of which date to a later time compared with the estimated date of Legendarium creations. These pigments include Prussian blue, pigments based on monoazo group and phthalocyanine blue. This contributes to the identification and localization of later interventions in the object under study, which were made both for the purpose of restoration and preservation.