A multimodal nonlinear optical microscope is a microscope capable of imaging in two or more nonlinear optical imaging modalities, such as second harmonic generation, two-photon excitation fluorescence, and coherent Raman imaging. These imaging modalities provide researchers with the means to image biological structures, responses, and chemical compositions, label-free, and are fast becoming invaluable tools of biomedical investigation. In the Lab for Laser Assisted Medical Physics and Engineering (LLAMPE), we seek to apply such microscopy for biomedical research and to demonstrate its utility in new areas. We also seek to demonstrate new technologies to improve performance, robustness, and general utility, and so we have built such a microscope and have been using it in various studies since construction.Firstly, my supervisor, Professor Sangeeta Murugkar, who has been incredibly helpful in her role as a mentor and advisor. Without her insight, encouragement, and feedback, none of this would have been possible.Secondly, I would like to thank current and former members of our research group, the lab for laser assisted medical physics and engineering (LLAMPE), who have contributed in many ways, and made working in our lab enjoyable and productive. This includes Justin R. Gagnon and Olivia Raiche-Tanner, who have contributed to the construction of new sections, have helped improve the performance of the nonlinear optical microscope over the years, and have helped with some of the studies discussed herein. Hamid Moradi, Camille April Le Quere, and Abrar Ahmad, who helped lay the initial foundation of the microscope, and Connor McNairn and Amiel Beausoleil-Morrison who have always been helpful in providing spontaneous Raman spectra from various samples. Each of these individuals have contributed directly to our lab and helped perform some of the studies mentioned in this dissertation.Thirdly, I would like to thank our collaborators and others who have contributed to our lab and research, without whom many of these studies would not have been possible, and whose contributions greatly improved the scope and importance of each.