The incorporation of large‐sized rare earth (RE) elements with high coordination characteristics into transition metal dichalcogenide (TMD) absorbers while preserving a high 1T phase content during post‐processing poses a significant challenge. To address this, a novel strategy involving the confinement of RE elements within the 1T‐MoS2 lattice via liquid plasma assistance, is proposed. This approach effectively mitigates the environmental impact on the 1T phase of MoS2, yielding a remarkable 1T phase content of 82.69% for Ce20‐D7 (20 wt.% Cerium trinitrate and 7 kV applied voltage). Combining experimental and theoretical investigations reveals that the multi‐orbital characteristics of RE elements facilitate hybridization between the RE‐4f and Mo‐4d orbitals on the MoS2 surface, leading to the occupation of weakly bound electrons in bonding orbitals with short‐distance motion, enhanced inter‐orbital electron‐electron interactions, and induced polarization loss. Notably, the results demonstrate that the Pr15‐D7 sample (15 wt.% praseodymium nitrate and 7 kV applied voltage) exhibits an effective absorption bandwidth (EAB) of 7.12 GHz at 2.6 mm, with a minimum reflection loss of ‐52.02 dB while the Ce20‐D7 sample achieves an EAB of 6.96 GHz at 2.7 mm. These findings provide valuable insights for the rational design and development of high‐performance TMD absorbers leveraging RE‐modified materials.