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Pure cellulose nanocrystal (CNC) aerogels with controlled 3D structures and inner pore architecture are printed using the direct ink write (DIW) technique. While traditional cellulosic aerogel processing approaches lack the ability to easily fabricate complete aerogel structures, DIW 3D printing followed by freeze drying can overcome this shortcoming and can produce CNC aerogels with minimal structural shrinkage or damage. The resultant products have great potential in applications such as tissue scaffold templates, drug delivery, packaging, etc., due to their inherent sustainability, biocompatibility, and biodegradability. Various 3D structures are successfully printed without support material, and the print quality can be improved with increasing CNC concentration and printing resolution. Dual pore CNC aerogel scaffolds are also successfully printed, where the customizable 3D structure and inner pore architecture can potentially enable advance CNC scaffold designs suited for specific cell integration requirements.