Vibrational spectroscopy and imaging promise molecular information that can be rapidly acquired without the need for specialized stains or dyes, thereby potentially simplifying and speeding up necessary analyses for interventions in many facets of modern day healthcare. The salient characteristics of vibrational spectroscopy for molecular analyses, using non-perturbative optical measurements, and employing computational analysis of data, are especially useful near the point of care as assessments can be made with fewer reagents, under pressure of time and accuracy while not requiring extensive specialized human expertise. Significant technological development has occurred and many seminal proof of concept studies have been conducted to demonstrate the utility and vast potential of spectroscopic methods. Accordingly, a number of studies have focused on pushing the fundamental performance limits of spectroscopic methods while others have focused on specific problems where the use of vibrational spectroscopy promises to change the standard of care. Despite this impressive progress, however, the application area is still maturing and rapidly evolving. A vast array of potential applications continues to be assessed while others need further technological developments. In this review, we focus on recent developments that demonstrate potential for point of care impact and major trends that can lead, in turn, to improved spectroscopic technology. We provide focused examples of “case studies” and major trends in spectroscopic analyses ranging from in vivo measurements to that of ex vivo bodily fluids to extracted and processed tissues. In each case, the uniting theme is that information to the clinician is enabled closer to the patient, allowing for a shorter time between identification of the need for analyses and availability of information that guides care.