The development of magnetocaloric effect (MCE) material is done in order to reduce the damage of the ozone layer caused by the chlorofluorocarbons (CFCs) emitted into the air. The research dealing with synthesis of magnetocaloric materials based of Ni-Al Heusler Alloy structure and by varying substitution some atoms of Ni with Fe and Al with Mn on Ni-Al Heusler Alloy structure to become Ni44Fe6Mn32Al18. Vacuum Arc Melting (VAM) equipment is used to form the alloys on vacuum condition and by flowing argon gas atmosphere and then followed by annealing process for 72 hours. X-Ray Diffraction (XRD) reveals that crystallite structure of material is observed. We define that Ni44Fe6 as X2, Mn25 as Y, and Al18Mn7 as Z. Based on the XRD result, we observed that the general formula X2YZ is not changed. The PERMAGRAF measurement revealed that there exists of magnetic hysterysis. The hysterysis show that the magnetic structures of the system undego evolution from diamagnetic to soft ferromagnetic material which all of the compound have the same crystallite structure. This evolution indicated that the change in the composition has led to changes the magnetic composition. Mn is the major element that gives strong magnetic properties to the sample. When Mn partially replaced position of Al, the sample became dominant to be influenced to improve their magnetic properties. In addition, substitution a part of Ni by Fe in the composition reveals a pinning of the domain walls in the sample.