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A quantitative non-destructive express method of determining fillers —kaolin and chalk— in paper was created using attenuated total reflectance Fourier transform infrared (ATR-FT-IR) spectroscopy in the mid-IR and far-IR region (3800–245 cm−1) combined with partial least squares (PLS) data analysis. Altogether, 30 two-component (cellulose pulp + kaolin and cellulose pulp + chalk) reference paper samples with known different filler concentrations and one reference paper sample without any fillers were prepared for calibration and validation. The reference values of filler concentrations in the prepared papers were determined by gravimetric analysis via dry ashing (for establishing accurate concentrations of fillers in paper) and ATR-FT-IR microspectroscopy (for evaluating homogeneity of the papers). Two-component (cellulose pulp + kaolin or cellulose pulp + chalk) PLS models were created with papers of different cellulose types and containing different amounts of fillers. The best model had root mean square errors of prediction (RMSEP) for determining the kaolin or chalk content in the two-component papers of 2.0 and 2.1 g/100 g, respectively. The performance indices were 90.4% and 92.9%, respectively. As a demonstration of practical applicability of the method, different papers from books, journals, etc. were analysed. It was concluded that the developed quantitative method is suitable for non-destructive express analysis of kaolin or chalk in paper. [ABSTRACT FROM AUTHOR]