The present work investigates quantitatively the effect of induced anisotropy axis on magnetostriction of Terfenol-D, exploring a possible method of tailoring flexibly magnetostriction for a particular purpose. It is found that the induced anisotropy axis shows significant effect on the initial domain state, magnetization process, and thus the magnetostriction. Magnetostriction behaviors for a specific induced anisotropy axis are discussed and compared with the experimental observations. The critical case for the expected 90° domain alignments has been also analyzed quantitatively. Diagrams of domain state evolutions are established, shining some light on understanding magnetostriction tunability and developing magnetostrictive material.