Due to society’s increasing energy demand and the push for technological innovation within key industries (e.g. consumer electronics and electric vehicles), major advancements in energy storage technology, specifically battery technology, are needed. While Li-ion batteries are currently regarded as one of the premier options for reusable energy storage, they are not as safe, environmentally-friendly, or cost-effective as currently researched alternatives. One promising alternative is the rechargeable Zn/MnO2 battery which offers many benefits such as high energy density, low cost, and the ability to use non-corrosive electrolytes. In addition, the cathode material, MnO2, can exist in a variety of crystal structures which will offer distinct pathways or mechanisms for Zn-ion transport. This project explores how the crystal structure of MnO2 influences the electrochemical reaction mechanisms and subsequent performance of the Zn/MnO2 battery. Three different phases of MnO2 (α, β, and δ) were synthesized hydrothermally for use as cathode materials. Coin cells consisting of a Zn metal anode, MnO2 cathode, and an aqueous ZnSO4 electrolyte were then assembled and cycled to determine the charge/discharge behaviors of the batteries. Finally, the results of this project will help identify optimal cathode materials for improving the electrochemical performance of Zn/MnO2 batteries.