Nanoparticle uniformity dictates the long-range order in colloidal crystals. Gold cubes of the same average size, but different CV, were crystallized under the same experimental conditions. (A, C, and E) For each sample, an SEM image of the crystal is shown with an Inset of individual nanoparticles. (B, D, and F) Fast Fourier transforms of many images (Insets) can be azimuthally averaged to quantitatively evaluate uniformity.