The development of new high temperature materials for coatings as well as structural components is an important topic to contribute to a higher efficiency and sustainability of e.g. gas turbine engines. One promising new class of high temperature materials are NiAl-based alloys. Within this study, the microstructure and microhardness of NiAl-Ta-Cr alloys with varying Cr and Ta content were investigated. Graded specimens were fabricated by laser-based directed energy deposition utilizing an in situ alloying approach by mixing elemental Ta and Cr as well as pre-alloyed NiAl powder. Thermodynamic calculations were performed to design the alloy compositions beforehand. Inductive preheating of the substrate was used to counter the challenge of cracking due to the high brittleness. The results show that the cracking decreases with increasing preheating temperature. However, even at 700 °C, the cracking cannot be fully eliminated. Scanning electron microscopy, X-ray diffraction and electron backscatter diffraction revealed the formation of the phases B2-NiAl, A2-Cr and C14-NiAlTa within NiAl-Ta and NiAl-Cr alloys. For NiAl-Ta-Cr compositions, deviations regarding the phase formation between calculation and experiment were observed. Maximum hardness values were achieved within the NiAl-Ta and NiAl-Ta-Cr systems for the eutectic compositions at 14 at.-% Ta with maximum values above 900 HV0.1.