As the application of Raman spectroscopy to study bone has grown over the past decade, making it a peer technology to FTIR spectroscopy, it has become critical to understand their complimentary roles. Recent technological advancements have allowed these techniques to collect grids of spectra in a spatially resolved fashion to generate compositional images. The advantage of imaging with these techniques is that it allows the heterogenous bone tissue composition to be resolved and quantified. In this review we compare, for non-experts in the field of vibrational spectroscopy, the instrumentation and underlying physical principles of FTIR imaging (FTIRI) and Raman imaging. Additionally, we discuss the strengths and limitations of FTIR and Raman spectroscopy, address sample preparation, and discuss outcomes to provide researchers insight into which techniques are best suited for a given research question. We then briefly discuss previous applications of FTIRI and Raman imaging to characterize bone tissue composition and relationships of compositional outcomes with mechanical performance. Finally, we discuss emerging technical developments in FTIRI and Raman imaging which provide new opportunities to identify changes in bone tissue composition with disease, age, and drug treatment.