The quantification of the plutonium mass in spent nuclear fuel assemblies is an important measurement for nuclear safeguards practitioners. A program is well underway to develop nondestructive assay instruments that, when combined, will be able to quantify the plutonium content of a spent nuclear fuel assembly. Each instrument will quantify a specific attribute of the spent fuel assembly, e.g., the fissile content. In this paper, we present a Monte Carlo-based method of estimating the mean and distribution of some assembly attributes. An MCNPX model of each instrument has been created, and the response of the instrument was simulated for a range of spent fuel assemblies with discrete parameters (e.g., burnup, initial enrichment, and cooling time). The Monte Carlo-based method interpolates between the modeled results for an instrument to emulate a response for parameters not explicitly modeled. We demonstrate the usefulness of this technique in applying the technique to six different instruments under investigation. The results show that this Monte Carlo-based method can be used to estimate the assembly attributes of a spent fuel assembly based upon the measured response from the instrument.