Experiments have been conducted on the electrical breakdown of high-purity water and water mixtures. The electrical regime of interest has been carefully defined and documented to consist of electrical impulses with approximately microsecond rise time and fall time greater than 65 microseconds, on approximately 81-square-centimeter-area planar electrodes with a dielectric gap of approximately one centimeter. The results of over 25,000 shots by a Marx generator have been distilled into database form in an Excel spreadsheet and analysis performed to try to find patterns or indirect evidence into the nature of the breakdown-initiation process. An extensive review of all the experiments, which had been conducted over eight years by the Naval Surface Warfare Center and which had been designed to find the largest water-breakdown fields, was conducted with the intention of delineating the physical factors that led to breakdown. A variety of theoretical models of breakdown initiation were compared to the data, until it became clear that many of the breakdowns were dominated by impurities of various sorts. An extensive study of old and new experiments led to a more detailed understanding of the phenomenology of impurity-dominated water breakdown (such as the process of "conditioning" the electrodes and hysteresis) and the proposal of a number of new experiments to further characterize the intrinsic role of electrode materials on determining high-electric-field dielectric breakdown in water. / Ph. D.