Photovoltaic technology has the potential to become a major source of power generation. The fabrication of solar cells has improved stepwise from one generation to the next. First generation solar cells, i.e. silicon-based solar cells, were grown by the Czochralski process using a single crystal of silicon. Thin film development started in the second generation of solar cells. Nanocrystal-based solar cells were later introduced as the third generation of solar cells. This chapter discusses the progressive development of research into solar cells from one generation to the next. The focus is on nanocrystal-based copper indium gallium selenide (CIGS) and copper indium selenide (CIS) solar cells because of their flexibility, light weight, low cost, long life and excellent outdoor stability. Methods for the synthesis of CIGS- and CIS-based solar cells are discussed in detail.