The aerospace and power generation industries have an increasing demand for high-temperature, highstrength materials. However, conventional materials typically lack sufficient fracture toughness and oxidation resistance at high temperatures. This study aims to enhance the high-temperature properties of Nb-Si-Ti alloys through ball milling. To analyze the effects of milling time, the progression of alloying is evaluated on the basis of XRD patterns and the microstructure of alloy powders. Spark plasma sintering (SPS) is employed to produce compacts, with thermodynamic modeling assisting in predicting phase fractions and sintering temperature ranges. The changes in the microstructure and variation in the mechanical properties due to the adjustment of the sintering temperature provide insights into the influence of Nb solid solution, Nb5Si3, and crystallite size within the compacts. By investigating the changes in the mechanical properties through strengthening mechanisms, such as precipitation strengthening, solid solution strengthening, and crystallite refinement, this study aims to verify the applicability of Nb-Si-Ti alloys in advanced material systems.