The crystallization of digitally encoded polyurethanes was studied by electron diffraction. A series of oligomers with different primary structures was analyzed in this work. They all form hydrogen-bonding-directed lamellar single crystals with a base-centered orthorhombic unit cell. Although crystal morphology was the same in all cases, the digital coding of the oligomers has a small influence on the intersheet distance in the crystals. The crystal lattices allow calculation of the volume occupied by one basic information unit, which is in the range 148-188 Å3. Interestingly, this volume is about 3× smaller than that occupied by a coded nucleotide in a DNA double helix. Furthermore, crystallization of blends of oligourethanes with different coded primary structures was investigated. Oligomers with drastically different monomer compositions form structures that are not cocrystals but more probably segregated crystals containing distinct domains of different composition.