Efficient storage of thermal energy can be greatly enhanced by the use of phase change materials (PCMs). The selection or development of a useful PCM requires careful consideration of many physical and chemical properties. In this review of our recent studies of PCMs, we show that linking the molecular structures of organic molecules to their physical properties can be used to focus attention on the most useful PCMs, including eutectic mixtures. Two of the major limitations concerning broader use of phase change materials are low thermal conductivity, especially for organic phase change materials, and suitable containment. We have addressed both issues in our recent investigations of novel form-stable composite PCMs with a freeze-cast matrix. The use of thorough experimental investigations, including cycling of materials hundreds or thousands of times through the melt-freeze processes, promotes our goals of advancing the use of PCMs for increased energy efficiency and sustainability.