The structural, electronic, and magnetic properties of novel functional magnetic intermetallics, in particular some of the most prominent magnetic Heusler alloys, have been reviewed with emphasis on their complex magnetic behavior and nonergodic glassy features, in contrast to the well‐known properties ofTi‐NiandNi‐Alshape memory alloys. Calculational procedures have been listed throughout the text and the theoretical results have been compared with experimental findings where possible. The thermodynamic properties of a few systems (Ni–Co–Mn–In), which undergo a structural phase transformation of displacive nature in conjunction with a metamagnetic first‐order phase transition, have been discussed in detail. The importance of such magnetostructural phase transition together with the so‐called thermodynamic (kinetic) arrest phenomenon for the appearance of a giant magnetocaloric effect has been underlined. The list of references should allow bridging the gap between shape memory alloys such asTi–Ni(including recentab initiocalculations that explain the rapid decrease of the martensitic transformation temperature with disorder) and the “exotic properties” of the magnetic intermetallics.