This work has been conducted to investigate the effect of accelerated ageing on the filler-free (control) handsheets and the ones having Precipitated Calcium Carbonate (PCC) and Zeolite (Clinoptilolite) fillers. The diagnosis approach of this work has been based onthe use of the techniques of attenuated total reflectanceFourier transform infrared spectroscopy (ATR-FTIR) and X-ray diffraction (XRD). The FTIR technique has allowed identifying the changes in cellulose components of hand-sheets. Likewise, the XRD technique has provided to diagnose the changes in crystallinity of the handsheets and fillers. The results found out that PCC and Zeolite fillers could be easily added to the structure of the paper network by changing various experimental variables. Thelossof C−O functional groups and the formation of carbonyl groups in handsheets has been analysed by accelerated ageing. Thespectroscopy results confirmed thatus age of zeolite filler has a retarding and structurally improving effect on the glycosidic linkages. Recent findings have been provided new insights into the role of the synergistic effect of the combination of PCC and zeolite fillers in the decelerating of certain ageing mechanism.