Structural engineering via the template method is efficient for micro‐nano assembling. However, only structural design and lack of composition control restrict their advanced application. To overcome this issue, applying a template to simultaneously realize the structural design and fine component control is highly desired, which has been ignored. In this study, a spinel‐shaped MoS2 heterostructure with controlled phase ratios of 1H and 2H phase is developed using the AlOOH template method. This work demonstrates that the MoS2 phase transition mechanism from 2H to 1T is substantially attributed to the close exposed crystal's surface and approximately accordant surface energy. The superiority and additional proof are provided based on density‐functional theory simulation, transmission electron microscope holography, etc. With an effective absorptance region of 6.3 GHz under a thickness of 1.4 mm, the reported samples present outstanding microwave absorption capacity. This is attributed to the beneficial coupled effect between the well‐designed structure and phase regulation. This work offers valuable insights into structural engineering and component regulation template methods.