Due to sequence binding constraints and a requirement for a TpA step for crosslinking, it is not possible to use pso-TFOs to target origami folded from commercially available scaffolds directly, e.g., M13mp18 or its derivatives. Our strategy therefore involved introducing a crosslinkable TFO target duplex sequence into the stem-loop hairpin(s) (HP) projected from the origami staples. This was achieved by extending the 3′ end of a specific origami staple(s) with a 32-nt sequence that folds intramolecularly into a 12-nt HP separated from the scaffold Crosslinking of multiple adjacent HPs was expected to form "super-staples" that further tether the TFO to the structure and increase the structural integrity of the origami. Functionalization is made possible by the attachment of cargo to the free 3′-end of the pso-TFO (shown as X in