This paper describes the combined use of voltammetry and electrode illumination during the anodic growth of Cu2S and CuInS2 films on copper substrates in sulfide containing KOH medium. The importance of compound stoichiometry in the two systems on the quality of the photoresponse was brought out in these experiments either by varying the positive potential limit (in the Cu-S case) or by In3+ ion addition tin the Cu-In-S case) during film growth. The in situ use of electrochemical quartz crystal microgravimetry and coulometry provided further insights into the mechanistic aspects of film growth in the two systems. Further, Raman spectroscopy evidence is presented in support of a new wurtzite-type structure for the CuInS2 films grown under galvanodynamic conditions.