High-resolution inkjet printing of a hydrophobic polymer surface (polystyrene, PS) was accomplished using a patterned coating of cellulose nanocrystals (CNCs) that prevents the ink from bleeding. A periodically crack-free, wrinkled (wavelength of around 850 nm) stamp was prepared by surface oxidation of an uniaxially stretched poly(dimethylsiloxane) elastomeric substrate and was used as a template to transfer aligned patterns of cellulose nanocrystals (CNCs) onto PS surfaces by wet stamping. The morphology of the aligned CNC coatings on PS was then compared with randomly deposited CNCs on PS using atomic force microscopy. The wettability of the CNCs and polymer surfaces with water and ink was measured and analyzed in the context of inkjet printing. This biomaterial coating technique enables high-resolution printing of modern water-based inks onto hydrophobic surfaces for applications in renewable packaging and printing of biomolecules for high throughput diagnostics. Further, with suitable modifications, the technology is scalable to roll-to-roll manufacturing for industrial flexo printing.