The growth, structure, and properties of two-dimensional boron nitride (BN) nanostructures synthesized by a thermal chemical vapor deposition method have been systematically investigated. Most of the BN nanosheets (BNNSs) were less than 5 nm in thickness, and their purity was confirmed by X-ray energy dispersive spectroscopy, X-ray photoelectron spectroscopy, electron energy loss spectroscopy, and Raman spectroscopy. The effects of the process variables on the morphology and roughness of the coatings were studied using atomic force microscopy and scanning electron microscopy. A smooth BN coating was obtained at 900 °C, while compact BNNS coatings composed of partially vertically aligned nanosheets could be achieved at 1000 °C and higher temperatures. These nanosheets were mostly separated and exhibited high surface area especially at higher synthesis temperatures. The nonwetting properties of the BNNS coatings were independent of the water pH and were examined by contact angle goniometry. The present results enable a convenient growth of pure BNNS coatings with controllable levels of water repellency, ranging from partial hydrophilicity to superhydrophobicity with contact angles exceeding 150°.