The overall aim of this thesis is to fill a specific methodological gap for the study of neurobiology. Our goal is to develop and apply a spectroscopic technique that can be used to study the living myelin of the peripheral nervous system. Just as modern scientists can appreciate the composition of a distant galaxy by the emission properties of the light that we receive from it, we likewise aim to glean information about living myelin biochemistry using quantifiable light principles. We suggest that the photophysical properties of myelin-incorporated solvatochromic dyes can be exploited to probe the biochemical composition of living myelin. To this end we analyze several potential dye candidates for maximum efficacy and consistency (Chapter 3). After demonstrating the superiority of Nile Red in these regards, we use this dye to probe the biochemical environment of early remyelination, both in-vitro and in-vivo, using high-resolution spectral confocal microscopy (Chapter 6). This combined work required the adaptation of a focal demyelination injury model to be amenable to cell graft therapy (Chapter 4), and also the development of a novel method of intravital imaging of the peripheral nervous system (Chapter 5). Our results demonstrate a consistent bi-phasic evolution of myelin spectra during early regeneration, both in-vitro and in-vivo. In total, this thesis presents a novel technique for probing the chemistry of PNS myelin with light, and is applicable to scenarios unworkable by existing methods of lipid chemical analysis, namely in the study of living nervous system.