Heusler alloys present a large group of binary, [1][2][3][4][5] ternary, [6][7][8][9][10] or quaternary [11][12][13][14] compounds with a wide variety of physical properties. [15][16][17][18] Thanks to their extensive tunability [19][20][21][22] based on their chemical composition, crystal, or electronic structure, [23][24][25][26][27][28][29] they attract interest in the fundamental and application approach. [30][31][32][33][34] Particularly, spin polarization, [33,35] superconductivity, [36][37][38][39] shape memory, [40][41][42][43][44][45] or magnetocaloric behavior [28,40,[46][47][48][49][50] have triggered significant interest in the experimental and theoretical perspective.Based on the chemical composition and the resulting properties, Heusler alloys, also known as full-Heusler alloys with the stoichiometry X 2 YZ, can be divided into several groups according to their physical properties. [51] Co 2 YZ-based Heusler can be considered the leading group of materials showing high spin polarization (P) or even half metallicity (P ¼ 100%). [52][53][54][55][56][57] However, theoretical and experimental studies point to the high sensitivity of spin polarization on the structural disorder. [58] Here, the L2 1 crystalline phase exhibits the highest structural ordering, essential for achieving the required spin polarization values. [59] In contrast, while the mutual exchange of the atoms on the Y-Z position (B2 disorder) has a low influence on the spin polarization values, the X-Y or X-Y-Z disorders (D0 3 or A2, respectively) may significantly decrease spin polarization values. [55,60,61] The presented disadvantage can be solved by a suitable chemical composition or a proper method of preparation of Heusler alloys. [62,63] Stoichiometric and off-stoichiometric Ni-Mn-Z- [64][65][66] and Ni-Fe-Z-based Heusler alloys [67][68][69] are well-known magnetocaloric, shape memory, or even magnetic shape memory materials. [70,71] The mentioned Heusler alloys undergo a structural transformation from a low-temperature martensitic phase to a high-temperature austenitic phase, [51,[64][65][66][72][73][74] which may significantly influence the magnetic entropy change ΔS M and the intensity of the magnetocaloric effect. [75,76] Additionally, Heusler alloys consist of cheap elements like Ni, Fe, Mn, Co, Ga, and In, and thus may be considered low-cost counterparts for typical magnetocaloric material based on Gd, Rh, or other rare-earth elements. [77][78][79][80][81] Another advantage of the Ni-Mn-Zand Ni-Fe-Z-based Heusler alloys consists in the tunability of their structural and magnetic properties. Depending on the