Urolithiasis is a prevalent, disturbing, and highly recurrent disease. Knowing the composition of a urinary stone is important for prevention purposes. Traditional urinary stone analysis methods need large stone fragments for analysis. However, the advancement of ureteroscopic lithotripsy (URSL) has resulted in micro-stone fragments and unapparently expelled urinary stone powder. In this study, we developed a micro-Raman spectroscopy (MRS) based diagnosis method for detecting micro-stones or stone powders in urine after URSL. In our experiment, urine samples of 10 ml each were collected from 12 patients over the fragmented stone site in the ureter after the URSL procedure. The post-URSL urine sediments extracted from urine were analyzed by MRS. The small urinary stones caught by grasping forceps were analyzed by both MRS and Fourier-transform infrared (FTIR) spectroscopy. We have identified common urinary stone compositions: calcium oxalate monohydrate (COM), calcium oxalate dihydrate (COD), dicalcium phosphate dihydrate (DCPD), calcium phosphate hydroxide (hydroxyl apatite or HAP), and uric acid, by using a 632.8 nm He-Ne laser for excitation, a 100x microscope objective lens for irradiation and collection, and a short photobleaching time for fluorescent background reduction. Thus, we developed an MRS-based method for analyzing the composition of urinary stone powders directly from the urine samples after the URSL procedure. This approach provides a quick and convenient method for urinary stone analysis.