The application of infrared and Raman spectroscopic techniques to the analysis of urinary calculi is reviewed and their relative efficiency and adaptability to routine analysis are discussed. Using the classification of urinary calculi based on their main constituents, infrared and Raman spectra of calcium oxalates, phosphates, uric acid, urates, and cystine are reported. Some characteristic bands are suggested as useful for analytical purposes. References to other constituents such as drugs are included. Although this review is aimed principally at human stones, it also extends to literature references dealing with urinary calculi from canine, feline, and equine animal species. © 1997 John Wiley & Sons, Inc. Biospectroscopy 3: 331–346, 1997