Recently, triplex motifs have been used as secondary structural elements capable of compacting dsDNA into various new DNA origami architectures. Such structures are assembled from designer scaffolds containing multiple distinct polypurine-polypyrimidine TFO target sequences folded by triplex-mediated crossover strand exchange. Our functionalization strategy could extend this design process, e.g., by attaching psoralen and other cargo to the crossover TFOs. The combination of such triplex technologies will result in a new generation of functionalized origami nanostructures that exhibit enhanced configurability and stability over those obtained with their duplex-only counterparts. This is likely to have most benefit with origami designed for use in biomedical science, where maintaining the structural integrity and function of the origami is paramount.