HfNbTaTiZr high-entropy alloy has wide application prospects as a biomedical material, and the use of laser additive manufacturing can solve the forming problems faced by the alloy. In view of the characteristics of the one-time forming of additive manufacturing methods, it is necessary to develop non-mechanical processing modification methods. In this paper, deep cryogenic treatment (DCT) is first applied to the modification of a HEA with BCC structure, then the post-processing method of DCT is combined with laser melting deposition (LMD) technology to successfully realize the coordinated improvement of forming and strength–ductility synergistic improvement in lightweight Hf_0.25NbTa_0.25TiZr alloy. The final tensile strength of the alloy after DCT treatment is 25% higher than that of the as-cast alloy and 11% higher than that of the as-deposited alloy, and the elongation is increased by 48% and 10%, respectively. In addition, DCT also achieves induced phase transition without additional deformation.