Previous strategies for selective placement of DNA origami (in some cases with controlled orientation) on lithographically patterned Si substrates leverage electrostatic interactions, with background passivation using a hydrophobic trimethylsilyl layer produced by hexamethyldisilane (HMDS). Here using the identified polypeptoid brush (PP3) with high DNA origami binding affinity, and a PMMA brush as the surface passivation layer for the background, surface chemical contrast nanopatterns with polypeptoid-modified circular patches of commensurate feature size are fabricated for selective binding of the 61 nm × 52 nm DNA origami nanostructures (Figure ). Previous studies on individual DNA origami placement and orientation on lithographically patterned surfaces have reported stringent deposition and rinsing conditions. Here using the PMMA-PP3 chemical contrast nanopattern, we are able to achieve a relatively high binding site occupancy of individual DNA origami without complicated deposition and rinsing protocols.