To realize the decoupling control of the dual corrector of liquid crystal (LC)–deformable mirror (DM) adaptive optics (AO) systems and prevent the loss of correction ability induced by coupling aberrations, a wavefront decoupling method based on DM eigenmodes was proposed. The coupling relationship of two correctors was studied, and the distribution of aberrations corrected using the DM and LC was investigated. First, a DM eigenmode matrix was derived according to the DM influence function. Then, aberrations were decomposed according to the Strehl ratio, and the projection of the LC response matrix on the DM eigenmode matrix, that is, the coupling term, was derived. Before using the LC corrector, the coupling item was eliminated for the decoupling of the two correctors, and the decoupling effect was verified through simulations. Finally, a 2 m telescope LC–DM AO system was developed to validate the proposed method. The simulation and experimental results showed that the root mean square of the DM-corrected residual after 55 eigenmodes’ correction was 0.09 μm. After decoupling correction, the resolution of the 700–1700 nm wide band improved from 1.1 to 1 times the diffraction limit, which is 1.2 times better than that obtained using the traditional Zernike mode correction.