Self-assembly of nanocrystals (NCs) into periodically ordered structures on multiple length scales and over large areas is crucial to the manufacture of NC-based devices. Here, we report an unusual yet universal approach to rapidly assembling hierarchically organized NC films that display highly periodic, tunable microscale stripe patterns over square centimeter areas while preserving the local superlattice structure. Our approach is based on a drying-driven dynamic assembly process occurring on a liquid surface with the stripe pattern formed by a new type of contact-line instability. Periodic ordering of NCs is realized on microscopic and nanoscopic scales simultaneously without the need of any specialized equipment or the application of external fields. The striped NC superlattice films obtained can be readily transferred to arbitrary substrates for device fabrication. The periodic structure imparts interesting modulation and anisotropy to the properties of such striped NC assemblies. This assembly approach is applicable to NCs with a variety of compositions, sizes, and shapes, offering a robust, inexpensive route for large-scale periodic patterning of NCs.