Abstract: The amounts of nuclear materials in the LiCl-KCl salt in pyroprocessing have to be analyzed to prevent the diversion of the nuclear material. An alternative method to the chemical analysis has been pursued, and laser-induced breakdown spectroscopy (LIBS) is one candidate. In the present work, an in situ and quantitative analysis method of electro-recovery (ER) salt was proposed and demonstrated by using LIBS combined with dipstick sampling. Two types of simulated salt samples were prepared: ER salt sample and salt obtained from the dipstick sampling, and pulsed neodymium-doped yttrium aluminum garnet (Nd:YAG) laser with a wavelength of 532 nm was focused on the salt to generate plasma. The plasma emission was measured by using an Echelle spectrometer with a resolution of 0.01 nm in conjunction with an Intensified Charge-Coupled Detector camera. The U and other rare earth peaks in the spectra were identified. The best Limit of Detection and Root Mean Square Error of Calibration of U were 38 ppm and 0.0203 wt%, respectively. Our work shows that the U in the pyroprocessing ER salt can be monitored with LIBS.