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We have demonstrated the fabrication of highly continuous and smooth CdSe semiconductor films containing self-assembled nanocrystals (NCs) using a simple, low cost solution-processed deposition technique. The impact of thermal annealing and ethanedithiol (EDT) treatment on oleate capped CdSe NCs films is illustrated. Post deposition EDT treatment enhances strong electron coupling between NCs by reducing the inter-particle distance, which enhances four orders of magnitude of photocurrent in the pn-device. Mild thermal annealing of NC films cause large redshift and significant broadening. Our findings suggest that NCs with short-range organic ligands are suitable for high-performance Thin-Film-Transistors and next generation high-efficiency photovoltaics. [ABSTRACT FROM AUTHOR]