This chapter describes the state-of-the-art in vibrational spectromicroscopy and imaging of metal carbonyl complexes in cells and tissues. It covers in detail the main spectroscopic techniques that make specific use of metal carbonyl bioprobes and which are currently employed in cellular imaging. These are, respectively, infrared (IR), Raman, and one instance of near-field microscopy. Of the vibrational microscopy techniques used to study metal carbonyl compounds, photothermal induced resonance (PTIR) undeniably provides the highest resolution, allowing measurements on subcellular structures. Numerous techniques are currently in use to obtain vibrational spectra of molecules. IR and Raman spectroscopy are implemented as microscopy techniques, for which the light delivery and collection optics are composed of fast lenses or objectives to allow focusing of the light beam to a small spot. Vibrational microscopy techniques, as a way to visualize cellular structures and dynamic processes in real time, are still in their early stages of development.