Biological materials found at a crime scene are crucially important evidence for forensic investigation because they provide contextual information about a crime and can be linked to the donor-individuals through combination with DNA analysis. Applications of vibrational spectroscopy to forensic biological analysis have been emerging because of its advantageous characteristics such as the non-destructivity, rapid measurement, and quantitative evaluation, compared to most current methods based on histological observation or biochemical techniques. This review presents an overview of recent developments in vibrational spectroscopy for forensic biological analysis. We also emphasize chemometric techniques, which can elicit reliable and advanced analytical outputs from highly complex spectral data from forensic biological materials. The analytical subjects addressed herein include body fluids, hair, soft tissue, bones, and bioagents. Promising applications for various analytical purposes in forensic biology are presented. Simultaneously, future avenues of study requiring further investigation are discussed.