Given tunable hybridization structures in solid solutions, fascinating electromagnetic (EM) properties can be achieved for regulating EM wave (EMW) absorption. Herein, a novel metal–organic cooperative interactions method is proposed to manipulate the vacancy, interstitial, substitutional, and heterointerface structures in molybdenum disulfide (MoS2) solid solution simultaneously, thence meeting the synergistic polarization loss on various point and face sites. Assisted by the coordination between Cu2+ and polydopamine (PDA), the effect of Cu modification on MoS2 is highly improved, which further lead to polarization loss on S vacancy, interstitial Cu, substitutional N, and heterointerface between carbon and MoS2. Contributing to the synergetic effect among multiple polarizations, the Cu/C@MoS2 solid solution exhibit ultrahigh EMW absorption performance, of which EMA with twice PDA delivers the effective absorption bandwidth of 7.12 GHz and minimum reflection loss of −48.22 dB (2.5 mm). The energy attenuation of Cu/C@MoS2 improved almost 266.7% and 222.2% than C@MoS2 and Cu@MoS2, respectively. Finally, this work reveals the structural dependency of solid solution materials of EMW absorption and establishes an entirely new polarization loss model.