The rejuvenation efficiency of aged bitumen is the main concern when developing rejuvenating agents. It is necessary to develop a method to assess the efficiency of rejuvenators using rheological parameters in the whole frequency region. To this end, the 2S2P1D micromechanics model is adopted to fit the entire G∗ master curves of various rejuvenated bitumen, and the influence of rejuvenator type/dosage and aging grade of bitumen on the whole G∗ master curve and chemical indices are investigated. Critical parameters for evaluating rejuvenation efficiency derived from viscoelastic models and chemical characterizations are proposed. Furthermore, the potential relationships between the rheological model-based parameters (E∞, δ, β, and τ) and chemical indices (carbonyl index CI and sulfoxide index SI) are explored. The results indicate that rejuvenators restore the δ, τ, CI, and SI values of aged bitumen towards the virgin bitumen level. The E∞ parameter is not applicable to evaluate the rejuvenation efficiency of engine-oil and naphthenic-oil rejuvenators, but the positive E∞R values of bio-oil and aromatic-oil rejuvenated bitumen are detected. All rejuvenators fail to restore the β parameter of aged bitumen. The τ and CI parameters are selected as critical evaluation indicators from the perspective of viscoelastic models and chemical characteristics. Linear correlations between all rheological parameters and chemical indices are observed and established.