Presented herein are the outcomes of an experimental test involving a pioneering portable-active interrogation system designed for the nondestructive detection of special nuclear materials (SNMs). The system relies on the threshold energy neutron analysis concept and incorporates a portable deuterium–deuterium (DD) neutron generator producing a particle intensity of 5 × 107 n/s, coupled with three arrays of tensioned metastable fluid detectors (TMFDs) to detect secondary neutrons from the fissile material. In the presence of the fissile material, prompt fission neutrons are emitted, with an average energy of approximately 2 MeV, and around 30% of these neutrons have energies above that of the DD neutron source (2.45 MeV). The detection of a statistically significant neutron population exceeding this threshold firmly indicates the presence of SNM. TMFDs exhibit high sensitivity in efficiently detecting neutrons above the threshold while adeptly discriminating against neutrons below the threshold as well as gamma rays. This unique feature allows the interrogation system to maintain a lightweight profile without necessitating substantial shielding materials. The validation experiments involved the placement of 70 or 140 g masses of U-235 within a 1 m3 inspection volume. Measurements were carried out over 30 min intervals, repeated numerous times, both with and without U-235, at a DD neutron source intensity of 8 × 105 n/sec. Experimental count rates with natural uranium (NU) are consistently above those without NU. The probability of detection (PD) and probability of false alarm (PFA) were assessed utilizing these count rates. The DD neutron source intensity and inspection time were normalized at 5 × 107 n/sec and 90 s, respectively. The results indicated a PD of approximately 74% and 98% for detecting 70 and 140 g of U-235, respectively, with a PFA of <5%. These promising outcomes align with the specified PD (>90%) and PFA (<5%) targets outlined in ANSI standards.