In this work, LaNi5 and LaNi3.94Al1.06 alloys were prepared by vacuum induction melting method. Then, samples were hydrogenated under 50 bar hydrogen gas pressure. The structural properties of samples, before and after hydrogenation, were investigated using X-ray diffraction (XRD) and energy dispersive spectroscopy (EDS). The results showed that all of the samples are single phase with a hexagonal crystal structure (CaCu5 type). The magnetic measurements indicated that as-prepared samples were weak ferromagnetic or paramagnetic which became ferromagnetic after the hydrogenation process. These variations were attributed to the decomposition of nickel magnetic phase from the alloys. Substitution of Al for Ni in the as-prepared sample reduces the magnetic susceptibility from 4.8−6 to 4.1 × 10−6 emu/g Oe. The Law of Approach to Saturation was used for investigating the magnetic anisotropy of the hydrogenated samples in high magnetic field. In the hydrogenated samples, magneto-crystalline anisotropy is increased when the Ni magnetic metal is replaced with the Al nonmagnetic inclusion. All of these measurements were carried out at room temperature.