Hydrophobic coatings are widely used in many fields, such as packing, textile, etc. However, hydrophobic coatings with the advantages of environmentally friendly, facile to prepare, non-toxic, easy to use and biocompatible are still rare and attractive. In this study, sustainable cellulose nanocrystal (CNCs) were employed as building blocks to construct superhydrophobic coatings. Superhydrophobic CNCs were facile prepared by anchoring octadecylamine on the surface of native hydrophilic CNC via the oxidization self-polymerization of tannic acid. The superhydrophobic CNCs can be well-dispersed in ethanol to form a spray, and superhydrophobic coatings on many materials could be obtained by spraying the superhydrophobic CNC ethanol dispersion at a low dosage about 1 g/m2. The facile prepared hydrophobic coatings made of modified CNC show good friction resistance and can be repeatedly washed without affecting the waterproof ability. Due to their non-toxicity, convenience, and durable properties, superhydrophobic CNCs are promising in a variety of fields, including waterproof paper-based packaging for express delivery, waterproof cloth, oil-water separation, and so on.