In this work, we aimed to analyze suspensions of cationic starch by adding 5 wt%, 7 wt%, and 10 wt% of bentonite as a bilayer coating on kraftliner paper (85 g/m2). The controls were doubly-wet-and-dry and uncoated kraftliner paper. In a coating machine, the formulations were applied until reaching a grammage of 15 g/m2 and then dried at 103 ± 2 °C. The test was carried out about pH, solids content, and viscosity of the suspensions. The physical characteristics of the coated papers were evaluated, as well as their ability to block water, water vapor, and oil/grease. We also analyzed with scanning electron microscopy, Raman spectroscopy, and Fourier transform infrared spectroscopy. The packaging, having a water contact angle of up to 78° and 189 g/m² for Cobb, showed a low resistance to water, which is further responsible for decreased mechanical resistance. Nevertheless, the coating did not change the permeability to water vapor, however, bentonite promoted a decrease in wettability and Cobb value of the paper. The addition of 7 wt% bentonite to the cationic starch matrix promoted high oil resistance with 12 for kit-oil, while 10 wt% bentonite promoted greater pencil hardness, with a value of 8H. Bentonite strength and cationic starch showed good interaction, increasing oil resistance.