Employing ab initio electronic structure calculations, we study a new class of magnetic Heusler compounds, which consist only of 3d transition metal atoms, namely, Fe2CrZ and Co2CrZ, where Z is an early 3d-metal, such as Sc, Ti or V. Although these compounds show a pseudogap and high spin polarization at the Fermi level, the so-called Slater–Pauling rule is not applicable to them. Co2CrTi and Co2CrV compounds present robust magnetic properties due to the short range magnetic exchange interactions and, thus, relatively high values of Curie temperature far above the room temperature. Moreover, these two compounds keep their magnetic properties upon B2 disorder that makes them very promising materials for spintronic and magnetoelectronic applications.