Utilizing the Watson-Crick base pairing mechanism [ 23 ] and the interconnection by Holliday junctions, [ 24,25 ] the robust DNA origami technique allows the formation of arbitrary 2D [ 4 ] and 3D nanostructures. [5][6][7][8][9][10][11][12][13][14][15][16][17] Functionalization of these nanostructures with biomolecules, fl uorophores, metal nanoparticles, or semiconductor quantum dots opens interesting opportunities for biomedical applications, [ 18,19 ] analytics and microscopy, [ 26,27 ] nanoelectronics, [ 28 ] or nanoplasmonics and nanophotonics. [19][20][21][22][29][30][31][32][33][34] However, not only isotropic aqueous dispersions or surfaces containing well-defi ned nanoobjects, [ 35 ] but also bulk materials may be targeted, where these objects exhibit a well-defi ned orientation or are arranged in an array with well-defi ned positions. For this purpose, self-organization on a micrometer scale or mesoscale would be very useful. Liquid crystals (LCs), ordered fl uids, are ideal candidates for bridging the gap between ordering on the sub-µm and µm length scales. LCs show a collective behavior of anisometric molecules or molecular aggregates: the resulting phenomena, like elastic behavior, surface alignment, or interaction with external electric and magnetic fi elds are described by characteristic lengths, which are typically in the µm range.[ 36 ] This is not only important for fl at panel displays, where LC fi lms with a thickness of a few µm are realigned by electric fi elds, but can also be used to control the alignment of rod-like or disk-like nanoparticles, for example, gold or semiconductor nanorods, carbon nanotubes,