Improving patients’ clinical outcomes requires many levels of examination, owing to the enormous complexities of human disease and healthcare delivery. Our understanding of disease also requires many different levels of observation. The human experience preconditions us to see the whole person and to relate to them as individuals, each with their own unique set of circumstances. Modern medicine seeks to apply many forms of intervention, including surgical resection, radiation and chemotherapy, and more recently, targeted drug therapy. In this forum, we are concerned with disease and pathophysiology, and how best to reach the site or sites of disease with targeted therapies. Monoclonal antibodies and their fragments have long held promise in targeting epitopes unique to diseased cells, e.g. cancer. Peptides and small molecule ligands that are capable of binding unique expressions of disease are increasingly the focus of drug discovery and development. This thesis focuses on development of radioligands for molecular imaging and therapy and novel strategies to improve their application to achieve greater success. These efforts are pursued in order to improve patient outcomes through more accurate and timely diagnosis, staging, and monitoring of treatment interventions using molecular imaging, and to more effectively treat disease using highly targeted therapies.