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Precipitated calcium carbonate (PCC) is a filler that is widely used for papermaking, and lime sludge is a special type of PCC recovered from the black liquor from kraft pulping. There has been some concern that lime sludge may interfere with the development of paper’s hydrophobicity in comparison with commercial PCC and ground calcium carbonate (GCC) due to the presence of impurities when alkyl ketene dimer (AKD) is used as the sizing additive. In this work, fillers with different particle size distributions were prepared, and the effects of particle composition on surface chemistry of fillers, adsorption for AKD, sizing degree of final paper sheets, and retention behavior of fillers were evaluated. The results showed that, through matching different particle size distributions for lime sludge fillers, the negative zeta potential decreased from -26.2 mV to -20.8 mV, the specific surface area decreased from 15.0 m2/g to 9.1 m2/g, and total pore volume decreased from 0.037 cm3/g to 0.026 cm3/g, which was favorable for the low adsorption for AKD. Consequently the sizing effect of filled paper was improved. Moreover, the retention rate also was increased by changing the particle size distribution of lime sludge.