We investigated how pulsed laser annealing can be applied to process thin films of colloidal nanocrystals (NCs) into interconnected nanostructures. We illustrate the relationship between incident laser fluence and changes in morphology of PbSe NC films relative to bulk-like PbSe films. We found that laser pulse fluences in the range of 30 to 200 mJ/cm2 create a processing window of opportunity where the NC film morphology goes through interesting transformations without large-scale coalescence of the NCs. NC coalescence can be mitigated by depositing a thin film of amorphous silicon (a-Si) on the NC film. Remarkably, pulsed laser annealing of the a-Si/PbSe NC films crystallized the silicon while NC morphology and translational order of the NC film are preserved. © 2011 American Chemical Society.