In the present work, the composite cross-linked were used to consolidate the dyed paper manuscripts. Nanocomposites of mesoporous silica nanoparticle (MPSNP)/polyvinyl alcohol (PVA) and cellulose nanofiber (CNF)/PVA, which have never been used before, have been evaluated for the consolidation process of the dyed paper manuscripts with madder extract. Three concentrations 1%, 3%, and 5% have been prepared. Analysis and investigation methods like scanning electron microscope (SEM), transmission electron microscope (TEM), dynamic light scattering analysis (DLS), X-Ray diffraction Analysis (XRD), atomic force microscope (AFM), Fourier transform infrared spectroscopy (FTIR) and total color difference (ΔE) by spectrophotometer have been used in order to characterize the prepared nano-sized composites and evaluate the treated dyed paper samples before and after the aging process. The results of surface morphology by SEM revealed the effectiveness of MPSNP/PVA core–shell nanocomposite at 5% in the consolidation process, where the improvement of properties of the aged dyed paper samples. The fibers of the treated paper became strong and appeared clearly. The result of ΔE measurements showed that the treated sample with MPSNP/PVA nanocomposite at 5% gave the lowest ΔE (5.22), while, the treated sample with CNF/PVA nanocomposite at 5% gave the highest ΔE value (11.66). Mechanical measurements (tensile strength and elongation) revealed the efficiency of MPSNP/PVA nanocomposite at 5% in the treatment of the aged dyed paper samples. The treated sample with the mentioned material gave tensile strength and elongation values of 84.8 N/nm2 and 1.736%, respectively. In contrast, the treated sample with CNF/PVA nanocomposite at 1% gave the lowest tensile strength and elongation values 38.2 N/nm2, and 1.166%, respectively. FTIR analysis revealed an increase was noticed in the CH2 stretching band (refers to the crystallinity of cellulose), where the intensity of the treated sample with MPSNP/PVA nanocomposite was at a 5% increase compared to the control sample. The FTIR results supported the results of mechanical measurements. The intensity of the CH2 stretching band, which refers to the crystallinity index of cellulose, was increased with the use of MPSNP/PVA nanocomposite at 3% and 5%, which explains the improvement in mechanical properties. This may be due to the nano-mineral particles, which improve the mechanical properties. Additionally, they reduce the effect of accelerated thermal aging on the cellulosic fibers and give them stability. The detailed analysis of analytical methods used for evaluation revealed the novelty of MPSNP/PVA nanocomposite, especially at 5%. It has a potential role in strengthening and improving different properties of the dyed paper manuscripts with madder extract.