Cellulose nanocrystals (CNCs) are a particularly appealing format of the natural biopolymer due to their exceptional strength, nanoscale dimensions, and needle-like shape anisotropy. However, CNCs are hydrophilic and hence their wettability makes them impractical for many coating applications, with various approaches using chemical functionalization to overcome this. Here we show that CNC-coated surfaces can be rendered hydrophobic by alignment of the native CNCs using a wrinkled template-mediated printing process. We present a novel and simple method allowing full release of the CNCs from the template and their permanent adsorption into fine patterns onto the surface, thus preventing CNC repositioning during wetting. The aligned CNCs induce strong pinning effects that capture and retain water droplets with high contact angle and large roll-off angles, without becoming susceptible to oil contamination. The fabrication process for these coatings could be achieved by large-scale printing, making them a practical and cost-effective solution to hydrophobic coatings from raw cellulosic materials.