Self-assembly provides the basis for a procedure used to organize millimeter-scale objects into regular, three-dimensional arrays ("crystals") with open structures. The individual components are designed and fabricated of polyurethane by molding; selected faces are coated with a thin film of liquid, metallic alloy. Under mild agitation in warm, aqueous potassium bromide solution, capillary forces between the films of alloy cause self-assembly. The structures of the resulting, self-assembled arrays are determined by structural features of the component parts: the three-dimensional shape of the components, the pattern of alloy on their surfaces, and the shape of the alloy-coated surfaces. Self-assembly of appropriately designed chiral pieces generates helices.