The investigation of natural aging of writing inks printed on paper using Raman spectroscopy was performed. Based on the obtained dependencies of the Raman peak intensities ratios on the exposure time, the dye degradation model was proposed. It was suggested that there are several competing bond breaking and bond forming reactions corresponding to the characteristic vibration frequencies of the dye molecule that simultaneously occur during ink aging process. Also we propose a methodology based on the study of the optical properties of paper, particularly changes in the fluorescence of optical brighteners included in its composition as well as the paper reflectivity using spectrophotometric methods. These results can be implemented to develop the novel and promising method of criminology.