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A novel Ti-Ni-Hf-Cu-Nb shape memory alloy has been developed by a new combinatorial alloy synthesis method, the Suspended Droplet Alloying. The influence of alloying elements on the transformation temperature, the microstructure and the shape memory effect of this alloy have also been studied. It was found that Cu has a greater negative influence on the transformation temperature of Ti-Ni-Hf-Cu_X alloys (about −5 K/at.%) than on the Ti-Ni-Cu_X alloys (−0.67 K/at.%). In addition, the negative effect intensifies with increasing Hf content. The transformation temperature rapidly decreases with increasing Nb composition in the Ti-Ni-Cu-Nb and Ti-Ni-Hf-Cu-Nb alloys, with the solid solution of Nb in the matrix being 1 at.%. A Ti-Ni-Cu-Hf-Nb alloy with high thermal cycle stability has been developed, where the alloying elements affect the transformation behaviour via altering the slipping energy and forming different types of precipitations.