Magnesium (Mg) and its alloys provide numerous unique benefits as potential resorptive biomaterials and present the very real possibility of replacing current metallic implant materials in a variety of roles. However, considerable research remains before Mg alloys may be accurately screened and used in vivo. Most critically, a more comprehensive understanding of the corrosion of Mg alloys in vitro is needed. This research program critically examined the types of in vitro experiments that may be performed on Mg alloys, investigated the numerous variables that affect Mg biodegradation when undertaking these experiments, explored the electrochemical performance of several biocompatible Mg alloys, and developed a novel process for producing ordered Mg structures. The benefits and drawbacks of a range of in vitro tests were first investigated. The key strengths and weaknesses of each test were identified and recommendations provided for their respective use in the quest to determine Mg alloy biodegradation. The most common variables applicable to all in vitro experiments were then explored in detail, and their effect on the biocorrosion of a number of Mg alloys was determined. Recommendations were then made for the appropriate control of the different experimental variables based on these findings. For the first time, the mechanistic control of Mg biodegradation by the microstructure of biocompatible alloys has been examined. This allows for greater understanding of the reasons for varied corrosion of alloys in bio-electrolytes, and is a step towards the effective design of Mg alloys for different bio-applications. A novel method to produce ordered Mg structures was developed, with relevant processing parameters investigated in light of their effect on biocorrosion and mechanical performance. Overall, the results and findings from this research further our understanding of the potential of Mg alloys as suitable biomaterials, and advance our knowledge of how to proceed towards the goal of using such alloys for biological applications.