We designed two types of X-shaped branched DNA nanostructures named X-motif and origami-binding motif for constituting DNA condensates (Figure ). The X-motifs have four branches with an identical selfcomplementary 4-nucleotide (nt) sticky end to form DNA condensates ; the origami-binding motifs have three branches with an identical self-complementary 4-nt sticky end to hybridize with the X-motifs, and one branch with 23-nt origami-binding sequence to bind with a 3D DNA origami. We constructed DNA condensates (Figure ) by annealing a solution containing 2.22 µM X-motif and 0.56 µM origami-binding motif (2.78 µM in total) from 95°C to room temperature; i.e., the molar ratio was X-motif : origami-binding motif = ~80% : ~20%. Experimental details are in the Experimental Section and Table of Supporting Information. Figure (in Supporting Information) shows that the DNA condensates fused when collided, indicating the instability of DNA condensates toward fusion.