The self-assembly of nanocrystals enables new classes of materials whose properties are controlled by the periodicities of the assembly, as well as by the size, shape and composition of the nanocrystals. While selfassembly of spherical nanoparticles has advanced significantly in the last decade, assembly of rod-shaped nanocrystals has seen limited progress due to the requirement of orientational order. Here, the parameters critically relevant to self-assembly are systematically quantified using a combination of diffraction and theoretical modeling; these highlight the importance of kinetics on orientational order. Through dryingmediated self-assembly we achieve unprecedented control over orientational order (up to 96% vertically oriented rods on 1cm 2 areas) on a wide range of substrates (ITO, PEDOT:PSS, Si 3 N 4 ). This opens new avenues for nanocrystal-based devices competitive with thin film devices, as problems of granularity can be tackled through crystallographic orientational control over macroscopic areas.Colloidal nanocrystals offer a potential route to realizing low-cost solution-processed electronic devices. In particular, with their size-tunable properties, single-crystallinity, and inexpensive synthesis, semiconductor nanoparticles could enable improved optoelectronic devices. To date, however, the performance of nanoparticle devices has been limited, in large part, by the number of interfaces that charge carriers encounter before they can be collected; each interface presents an opportunity for recombination and subsequent charge loss or