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An investigation is presented into the effect of the long‐range order on the optoelectronic properties of PbS quantum dot (QD) superlattices, which form mesocrystals, for potential use in photodetector applications. By self‐assembly of QD nanocrystals on an Si/SiOx substrate, a highly ordered and densely packed PbS QD superlattice with a microscale size is obtained. The results demonstrate that annealing...