1 Introduction The production of hierarchically structured materials is driving many recent advances in the fields of photonics,[1] electronics,[2] catalysis,[3] sensing,[4] and nanomedicine.[5] The self-assembly of nanocrystals into crystalline lattices constitutes a promising bottom-up route to such metamaterials, as it permits to tune the functional emergent properties of the outcoming supercrystals via engineering of the individual building blocks.[6] While recent improvements in the...