Chitin is the second most abundant biopolymer in nature and has tremendous potential in renewable materials for packaging, energy storage, reinforced composites, and biomedical engineering. Despite attractive properties, including biodegradability, antibacterial activity, and high strength, chitin is not utilized widely due to strong molecular interactions, which make solubilization and processing difficult. We report a high pressure homogenization route to produce pure chitin nanofibers (ChNFs) starting with a mildly acidic aqueous dispersion of purified crab alpha-chitin. The well-dispersed ChNFs with diameter similar to 20 nm do not form strong network structures under conditions explored herein and can be directly processed into useful materials, bypassing the need to dissolve the chitin. Dried ChNFs form pure self-standing chitin films with the lowest to-date reported O-2 and CO2 permeabilities of 0.006 and 0.018 barrer, respectively. Combined with high flexibility and optical transparency, these materials are ideal candidates for sustainable barrier packaging.