The DNA condensate comprises two types of X-shaped DNA nanostructures: an X-motif and an origamibinding motif (Figure ). Because the 3D DNA origami has some condensate-binding tags (Figure ), a DNA-origami-coated DNA condensate (hereafter 'coated DNA condensate') can be formed (Figures 1c and 1e(i)). By responding to the input of origami-connecting DNAs, the DNA origami coating switches to being more solid by connecting the 3D DNA origami (Figures and(ii)), resulting in a DNA-origami-armored DNA condensate (hereafter 'armored DNA condensate'). We report that the armored DNA condensates successfully prevented their fusion, although the coated DNA condensates only achieved insufficient fusion prevention. Furthermore, we demonstrate that the armored DNA condensates show molecular selective semipermeability. This DNA origami-based coating strategy will provide an effective approach to functionalizing and regulating DNA condensates.