We constructed 'coated' DNA condensates by mixing the 3D DNA origami and the 'binders' with the DNA condensate solution above (Figure ; Experimental Section). Figure shows a typical confocal laser scanning microscopy (CLSM) image of a coated DNA condensate, showing a core-shell structure of the DNA condensate (magenta) coated with the 3D DNA origami (green). To investigate the effect of the affinity and shape of the 3D DNA origami on the coating efficiency, we constructed some 3D DNA origami with different binding valences and positions. First, the condensate-binding tags were placed only on one face of the 3D DNA origami (one-sided binding design) (Figure ). Figure shows CLSM images and the fluorescent intensity profiles of the 3D DNA origami coating the DNA condensates. DNA origami with 12 and 20 condensate-binding tags more efficiently accumulated on the surface of DNA condensates than 6 condensatebinding tags. For comparison, we tested another DNA origami design with condensate-binding tags on both faces of the DNA origami (both-sided binding design) (Figure ). In the case of the both-sided binding design, 3D DNA origami penetrated inside the DNA condensate more than in the case of the one-sided binding design (Figure ). In addition, we constructed a 2D DNA origami with a flatter structure (see Figures and, Supplementary Note S1, Tables S6-S8, and Experimental Section) for comparison. Figure shows the results of coating DNA condensates with the 2D DNA origami, indicating that many 2D DNA origami penetrated inside the DNA condensate in both cases of one-and both-sided binding designs, similar to the both-sided binding design of the 3D DNA origami.