High entropy alloys (HEAs) represent an interesting alloying strategy that can yield exceptional performance properties needed across a variety of technology applications, including hydrogen storage. Examples include ultra-high volumetric capacity materials (BCC alloys → FCC dihydrides) with improved thermodynamics relative to conventional high-capacity metal hydrides (like MgH2), but still further destabilization is needed to reduce operating temperature and increase systems-level capacity. In this work, we demonstrate efficient hydride destabilization strategies by synthesizing two new Al0.05(TiVNb)0.95-xMox (x=0.05, 0.10) compositions. We specifically evaluate the effect of Molybdenum (Mo) addition on the phase structure, microstructure, hydrogen absorption and desorption properties. Both alloys crystallize in a bcc structure with decreasing lattice parameters as the Mo content increases. The alloys can rapidly absorb hydrogen at 25 °C with capacities of 1.78 H/M (2.79 wt.%) and 1.79 H/M (2.75 wt.%) with increasing Mo content. Pressure-composition-isotherms suggest a two-step reaction for hydrogen absorption to a final fcc dihydride phase. The experiments demonstrate that increasing Mo content results in a significant hydride destabilization, which is consistent with predictions from a gradient boosting tree datadriven model for metal hydride thermodynamics. Furthermore, improved desorption properties with increasing Mo content and reversibility were observed by in situ synchrotron X-ray diffraction, in situ neutron diffraction, and thermal desorption spectroscopy.