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Optoelectronic devices incorporating semiconducting nanocrystals are promising for many potential applications. Nanocrystals whose size is below the exciton Bohr radius have optical absorption and emission that is tunable with size, due to the quantum confinement of the charge carriers. However, the same confinement that yields these optical properties also makes electrical conduction in a film of nanocrystals occur via tunneling, due to the high energy barrier between nanocrystals. Hence, the extraction of photo-generated charge carriers presents a significant challenge. Several approaches to optimizing the reliability and efficiency of optoelectronic devices using semiconducting nanocrystals are explored herein. Force microscopy is used to investigate charge behavior in nanocrystal films. Plasmonic structures are lithographically defined to enhance electric field and thus charge collection efficiency in two-electrode nanocrystal devices illuminated at plasmonically resonant wavelengths. Graphene substrates are shown to couple electronically with nanocrystal films, improving device conduction while maintaining carrier quantum confinement within the nanocrystal. And finally, the occupancy of charge carrier traps is shown to both directly impact the temperature-dependent photocurrent behavior, and be tunable using a combination of illumination and electric field treatments. Trap population manipulation is robustly demonstrated and verified using a variety of wavelength, intensity, an