The slowing-down-time method for the nondestructive assay of light water reactor (LWR) spent fuel is under development at Rensselaer Polytechnic Institute. A series of assay measurements of an LWR fuel assembly replica were carried out at the Rensselaer lead slowing-down-time spectrometer facility by using 238U and 232Th threshold fission detectors and 235U and 239Pu probe chambers. An assay model relating the assay signal and the signals of the probe chambers to the unknown masses of the fissile isotopes in the fuel assembly was developed. The probe chamber data were used to provide individual fission counting spectra of 235U and 239Pu inside the fuel assembly and to simulate spent-fuel assay signals. The fissile isotopic contents of the fuel were determined to better than 1%. Monte Carlo analyses were performed to simulate the experimental measurements, determine certain parameters of the assay system, and investigate the effect of the fuel assembly and hydrogen impurities on the performance of the system. The broadened resolution of the system caused by the presence of the fuel was still found to be sufficient for the accurate and separate assay of the uranium and plutonium fissiles in spent fuel.