An electrolytic cell was designed, built, and tested with several proof-of-concept experiments in which Zircaloy material was charged with hydrogen in order to generate zirconium hydride formations. The Electrolytic Charging with Hydrogen and a Thermal Gradient (ECH-TG) system has the ability to generate static 20°C to 120°C temperatures for a H2SO4 and H2O bath for isothermal experiment conditions. This system was designed to accommodate a molten salt bath in future experiments to achieve higher isothermal temperatures. Additionally, the design accommodates a cartridge heater, which when placed on the inside of the sample tube, can be set at temperatures up to 350 °C and create a thermal gradient across the sample. Finally, a custom LABVIEW VI, L2.vi, was developed to control components and record data during experimentation. This program, along with web cameras and the commercial StirPC software package, enables remote operation for extended periods of time with only minor maintenance during an experiment. While proving the concept for this design, 19 experiments where performed, which form the basis for a future parametric study. Initial results indicate formations of zirconium hydrides which formed rim structures between 8.690 +/- 0.982 μm and 12.365 +/- 0.635 μm thick. These electrolytically produced rims were compared with hydrides formed under a previous vapor diffusion experiment via Scanning Electron Microscope (SEM) imaging and Energy dispersive X-ray Spectroscopy (EDS) analysis. While the existing vapor diffusion method formed gradients of zirconium hydride, it failed to produce the gradient in the correct direction and also failed to create a hydride rim. The successful use of the ECH-TG system to create said rim, and some of the methods used to direct that rim to the OD of the tube can be used for future work with the vapor diffusion method in order to create zirconium hydrides of the correct geometry. The procedures and apparatus created for this project represent a reliable method for creating zirconium hydride rim structures.