We describe for the first time the crystallization in thin films of a DNA copolymer composed of a low molecular weight chitosan backbone to which a sequence of nucleic acids is grafted (chitosan-g-ssDNA). As assessed by atomic force microscopy, optical microscopy and spectroscopy, crystallization occurs due to intermolecular hydrogen bonding in which the nucleic acid strands engage. The morphology of the crystals depends on the affinity for the surface of the polymer segments that compose the DNA copolymer hybrid. The nucleic acids adsorb on mica and silica on which side-branched structures are observed whereas chitosan interacts preferentially with gold, and dendritic crystals are assembled. Attenuated total reflectance infrared spectroscopy supports the high ordering of the structure and the establishment of strong intermolecular interactions by hydrogen bonding.