A portable In-Field Alpha Spectrometry (IFAS) system was developed to support on-site uranium enrichment determination for samples taken at facilities working with gaseous UF6. It consists of a modified commercial alpha spectrometer, a vacuum pump, a laptop computer, and associated connectors and cables. The IFAS uses specially designed Single-Use Destructive Assay (SUDA) samplers to capture gaseous UF6 and convert and store it as UO2F2 in a thin-film zeolite. To examine the quantitative performance of the IFAS system a large number of replicate SUDA samples was acquired for natural uranium (NU, 0.72 wt%, 23 samples), low enriched uranium 1 (LEU1, 2.33 wt% 235U, 10 samples), and low enriched uranium 2 (LEU2, 4.62 wt% 235U, 10 samples). The standard deviation (SD) values for uranium enrichment determination with the IFAS for NU, LEU1, and LEU2, in 20-hour assays, were 0.037 wt% 235U, 0.063 wt% 235U, and 0.072 wt% 235U, respectively. A separate analysis suggests that comparable SD values can be achieved in less time, approximately 8–10 h. For context, these SD values are well below the International Atomic Energy Agency’s International Target Values for the determination of uranium enrichment in non-destructive assay measurements.