The aim of this study was to optimize the modification of Egyptian kaolinite for application in paper coating. The study focused on four modification methods; sedimentation process, chemical bleaching, calcination, and dealumination. The effect of these methods on the structure of kaolinite was studied using X-ray fluorescence (XRF), X-ray diffractometer (XRD), Fourier transform infrared spectrometer analysis, and field emission SEM. The original and modified kaolinites were applied in paper coating mixtures. The results of XRF analysis showed that the Fe2O3 and TiO2 in Egyptian kaolinite were reduced chemically via sodium dithionite from 0.41% to 0.25% and 2.20% to 2.00%, respectively. Calcination at 900°C, followed by acid activation and bleaching, showed a further decrease in Fe2O3 and TiO2 impurities to 0.012 and 1.45 (wt%), respectively. XRD results revealed that all characteristics reflection of kaolinite disappeared upon calcination. SEM investigation showed a significant reduction in kaolinite particle size. Calcination and dealumination of kaolinite did not improve coated paper roughness, while air permeance and optical properties significantly increased in comparison with commercial kaolinite. In addition, a significant improvement was observed in coated paper mechanical properties including burst, tensile strength, stretch, and tensile energy absorption with respect to original and commercial kaolinite. In contrast, the kaolinite fraction <2 µm highly improved paper gloss, print density, and print gloss, more than calcined kaolinite and its modified pigments. In conclusion, dealumination of calcined kaolinite did not show any further change in all coated paper properties compared to the calcined ones.