Carbon black filled natural rubber (CB/NR) is a paradigm of nanocomposite materials with high performances. However, the mechanism for the nonlinear Payne effect is still not fully clear. CB gel (CBG) network embedded in the entanglement rubber matrix is supposed to be crucial for the reinforcement and viscoelastic nonlinearity. In this paper, we report for the first time the preparation of bulk CBGs by extracting the highly filled compounds in toluene and the systematic study of their viscoelastic behaviors. The CBG obtained from highly filled compounds with CB loadings from 40 to 70 phr has almost identical microstructure and composition, containing 40 wt % inextractable rubber fractions, among which similar to 12 wt % is glassy. Dynamic rheological studies show that the Payne effect of the CBG network is frequency independent and highly resilient, exhibiting an unjamming characteristic. On the other hand, the Payne effect of highly filled compounds is determined by the coupling between the breakdown of CBG network and the frequency-dependent chain disentanglement of extractable rubber fractions. This work provides new insights into the Payne effect of CB filled NR and should merit designing other rubbery nanocomposites with high performances and functions.