A test experiment to polarize tritium nuclei to develop a polarized deuterium-tritium (D-T) laser fusion concept is proposed in which a ferromagnetic complex with a high internal magnetic field is used to polarize tritium nuclei on physisorbed D-T molecules with an internal β-decay heat load in a D-T target. Heteronuclear hydrogen deuteride (HD) is used to conduct the measurements herein instead of as in typical D-T–based experiments. As proof-of-concept experimentation, the adsorption and desorption characteristics of HD are examined on Prussian blue ferromagnetic analogue Ni3[Fe(CN)6]2 at temperatures of 77 K and around 23 K. Nuclear magnetic resonance (NMR) analysis of the ferromagnetic complex-mediated adsorption of HD onto activated carbon pellets at 10 K is conducted step by step using a multilocular probe cell that had been simplified to give a single-tube probe cell. The resulting 1H NMR spectra are compared with 19F NMR spectra obtained for reference on a Kel-F probe cell wall. Slight differences between the calculated NMR frequency from the gyromagnetic ratio and the actually observed NMR frequency are also discussed.