Methods of improving low-cost Cu2O|ZnO heterojunction diodes fabricated through galvanostatic deposition of Cu2O are presented. Improved processing parameters responsible for maximizing built-in voltage (Vbi) are determined. The relationship between pH, deposition current, temperature, and diode quality is analyzed and a process window for optimal Cu2O deposition on ZnO is obtained with a pH range between 12.0 and 12.1 and a current density range which is determined by the effect of both pH and deposition current (Jdep) on grain size. The pH window is found to be narrower than previously reported1 and much narrower than the processing window for the deposition of Cu2O films. A two-step approach deposition based on the use of different Jdep is presented for the first time. A Vbi of 0.6 V is achieved, which is the highest reported for cells produced using low temperature processing routes involving electrodeposition and reactive sputtering.