Optical techniques hold great potential to detect and monitor disease states as they are a fast, non‐invasive toolkit. Raman spectroscopy (RS) in particular is a powerful label‐free method capable of quantifying the biomolecular content of tissues. Still, spontaneous Raman scattering lacks information about tissue morphology due to its inability to rapidly assess a large field of view. Optical Coherence Tomography (OCT) is an interferometric optical method capable of fast, depth‐resolved imaging of tissue morphology, but lacks detailed molecular contrast. In many cases, pairing label‐free techniques into multimodal systems allows for a more diverse field of applications. Integrating RS and OCT into a single instrument allows for both structural imaging and biochemical interrogation of tissues and therefore offers a more comprehensive means for clinical diagnosis. This review summarizes the efforts made to date toward combining spontaneous RS‐OCT instrumentation for biomedical analysis, including insights into primary design considerations and data interpretation.