This perspective talk focuses on the history and status of electrodeposition for preparing thin films of inorganic and organic semiconductors, metal/semiconductor junctions, or even nanocomposite materials containing different phases. The use of light brings an added dimension and versatility to the preparative strategy. Variants on the basic cathodic or anodic deposition protocols will be elaborated as are approaches that rely on the initial deposition and stripping of a precursor layer. Another topic is operando compositional analysis of the depositing layers using a combination of electrochemical techniques with other complementary probes such as spectroelectrochemistry, electrochemical quart crystal microgravimetry (EQCM), and AC impedance spectroscopy. Finally, state-of-the art and future challenges will be discussed using examples drawn from the author’s and collaborators’ laboratories.