AbstractNew iron(III)99Mo-molybdate(VI) gels (Fe99Mo) of high Mo content were prepared by the precipitation/filtration method.99Mo–MoO3dissolved in NaOH was added to aqueous solutions of Fe(NO3)3at Mo/Fe mole fractions ~2.21 and 1.99 with continuous stirring at ambient room temperature. Two different Fe99Mo were precipitated from the mixed solutions adjusted at pH 2 and 4.7. The amount of water of hydration increased with the increasing the gel settling time and pH of the mixed solution. The matrices were characterized by radiometric, XRD, SEM, XRF, FT-IR, TGA, and DTA measurements. Small chromatographic columns of 2.0 g Fe99Mo containing ≥800 mg Mo tagged with 740 MBq99Mo were eluted with 5 mL saline solution. Highly reproducible99mTc elution indices suitable for preparation of99Mo/99mTc generators were achieved from generator supported with 0.5 g Al2O3filter. Elution performance of99mTc radionuclide was highly dependent on the gel structural properties.