Hydrogen (H2) storage has attracted the greatest attention in the contemporary day because of the shortage of fuel. The water splitting is considered less cost-effective and lead-free energy production by the photocatalytic process to produce hydrogen as a fuel for vehicles, petroleum refining, Pharmaceuticals, and glass purification. Perovskite materials play a vital role in H2 storage and production applications. The density functional theory (DFT) using the CASTEP code is used to study the various structural, electrical, optical, mechanical, and hydrogen (H2) capacity properties of ARH3 (A = K, Li, Rb; RSr, Ca) compounds. The compounds under investigations are optimized in the cubic structure; for ARH3 (A = K, Li, Rb; RSr, Ca), the optimized lattice constants are 3.924, 4.302, 4.559, 4.817, 4.647, and 4.884 Å, respectively. Since these hydrides are thermally stable, their formation energy is exhibited negative values. ARH3 may find usage in H2 storage applications due to its high gravimetric H2 storage densities (6.042 and 3.678 wt% for LiCaH3 and KCaH3, respectively). Furthermore, band gaps of 2.71, 2.38, 3.27, 2.73, 1.85, and 2.83 eV for ARH3 (A = K, Li, Rb; RCa, Sr) respectively, confirm the semiconductor behavior. These substances satisfy born stability criteria due to its mechanical parameters which derived from elastic constant values such as Pugh's ratio and modulus. Additionally, Pugh's ratio and Cauchy pressure demonstrate that, in contrast to other compounds, the KCaH3 compound has a ductile character (0.29). According to our analyses, studied compounds are observed a potential candidate for hydrogen storage devices.