Conventional methods of converting energy into mechanical work often involve a tedious, complex, and inefficient process. These limitations pose a barrier to the development of sustainable energy-conversion systems, especially in regards to environmentally benign conversion. However, recent advances in photomechanical crystals derived from photoswitch molecules offer an efficacious and promising alternative. Among these, diarylethene (DAE) compounds have emerged as an excellent candidate due to their high stability, photon-induced reversibility, and robust photo responsiveness. This study aims to synthesize, characterize and evaluate the photomechanical behavior of diarylethene-based crystals. This was accomplished in two phases. The first phase involved the synthesis of a variety of well-established diarylethenes, as well as novel but computationally promising candidates. The synthesized compounds underwent characterization using proton and carbon-13 nuclear magnetic resonance (NMR) spectroscopy. In the second phase, both open and closed isomers of the DAEs were crystallized in order to obtain their respective X-ray diffraction (XRD) patterns. High-intensity photoreactors were utilized to induce switching between the open and closed forms of the DAEs. Finally, single crystal X-ray diffraction analysis enabled visualization of the three-dimensional structures and crystal lattices of each isomeric form, which would become crucial in determining the mechanical response of each crystal. Once a comprehensive library of crystals and corresponding data was established, it was to be shared with collaborators at the University of California, Riverside (UCR) and the University of Colorado Boulder (CU Boulder) for further crystallographic and photomechanical study, as well as the exploration of potential applications.