Structural polysaccharide nanocrystals (NCs) including cellulose nanocrystal have attracted attention. In order to broaden the range of application of the NCs, we can take advantage of their original characteristics by establishing simple and reasonable processing methods. We here demonstrate a micropatterning of animal cellular adhesion by inkjet printing of aqueous dispersions of cytocompatible chitinous NCs onto cellophane films. We display how to regulate the deposition form and two-dimensional shape of the chitinous NC micromoldings using a research inkjet printer. Adhesive capability of mouse fibroblasts onto the chitinous substrates was greatly improved by alkali deacetylation. The deacetylated products remained rod-like nanostructures, but the original chitin crystal form changed to that of chitosan by an intensive deacetylation. The adhered cells could be recovered glycolytically. The chitinous micropatterning substrates can be utilized for biomedical applications such as controlling of cellular shapes, precise monitoring molecular events in biochemistry, and drug screening.