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In this work, pure Nb, Nb5Si3 and Laves Cr2Nb compound powders were used as raw materials to prepare Nb-Si- Cr tary alloys by spark plasma sintering (SPS). A comprehensive estimation of the microstructure and properties, including room temperature fracture toughness, high temperature strength and oxidation resistance, of the Nb-Si-Cr tary alloys as a function of the Nb/Nb5Si3/Cr2Nb phase volume fraction combinations was conducted. The results showed that Nb-Si-Cr tary samples with the relative density larger than 98.42% were obtained by SPS processing, and the samples all consisted of Nb, Nb5Si3 and Cr2Nb phases that were distributed homogeneously. The fracture toughness KQ of the Nb/Nb5Si3/Cr2Nb microstructure, which was dominated by the Nb phase, naturally increased with the Nb fraction. As expected, the room-temperature Vickers hardness and the high-temperature strength of the bulk alloys increased monotonically with the increasing of the stiffening Nb5Si3 fraction. Interestingly, the binary Cr2Nb phase played a positive role in the high temperature strength and oxidation resistance. Finally, the fracture modes of the typical Nb/Nb5Si3/Cr2Nb microstructures under bending and compression conditions at room and high temperatures as well as the oxidation mechanism are described and discussed.