A semiconductor nanocrystal film is a unique class of nanocomposite, whose collective properties are determined by those of its constituents. Colloidal synthetic methods offer precise size control and finely tuned optical properties via quantum confinement, while recent improvements in charge transport through films have led to a variety of optoelectronic applications. However, understanding the role of defects and impurities in doping, crucial for optimizing device performance, has remained more elusive. In this perspective, we review recent progress in understanding and controlling the doping of semiconductor nanocrystal thin films, with a special focus on its relevance to photovoltaic applications. We highlight an array of postsynthetic techniques based on stoichiometric control, metal impurity incorporation, and electrochemical charging. We conclude with a review of the state of the art for nanocrystal photovoltaics, and propose the use of controlled doping and charge balance as a pathway to higher device efficiencies.