Bioorthogonal chemistry is a burgeoning area of study that has innumerable applications. This dissertation describes applications of bioorthogonal chemistry to solve problems in the fields of imaging and metal uncaging. We first consider hyperpolarized magnetic resonance, a powerful tool in clinical and biochemical imaging that suffers from short signal lifetimes, which are typically less than a minute for many common molecular probes. Bioorthogonal handles such as azides and tetrazines are shown to be a viable, highly generalized approach to overcome these lifetime limitations in a variety of molecular probes. Additionally, in the field of inorganic chemistry, we hypothesize the potential use of bioorthogonal “click” reaction toward the development of a novel metal uncaging strategy. These innovative demonstrations of bioorthogonal chemistry highlight their potential in diverse areas of study.