Pre-alloyed Al-Li powders having high Li content were fabricated using thermal dehydrogenation of LiH. This, together with a rapid solidification process (RSP), led to strong suppression of the vaporization of Li. The uniform distribution of the Li present in the Al matrix was proved by confirming the random arrangement of δ'-AlLi precipitates seen in the microscopic images in the qualitative analysis. Spectroscopic analysis provided quantitative results for the concentration of Li. The dehydrogenation from LiH to Li was determined by H/O/N measurement, density reduction, and thermal analysis. Herein, we present that Al-Li powders with pre-determined 3.45 wt.% Li, can be prepared via thermal dehydrogenation with 5.00 wt.% LiH (4.37 wt.% Li), and that the resulting material could be used in high-performance powder metallurgical (P/M) applications for aircraft and aerospace structures.