Making full use of the interface modulation-induced interface polarization is an effective strategy to achieve excellent microwave absorption (MA). In this study, we develop an interfacial modulation strategy for achieving this goal in the commonly reported dielectric carbon nanotubes@polyaniline (CNTs@PANi) hybrid microwave absorber by optimizing the CNT nanocore structure. The heterogeneous interfaces from PANi and CNTs can be well regulated by longitudinal unzipping of the walls of CNTs to form 1D CNT- and 3D CNT-bridged graphene nanoribbons and 2D graphene nanoribbons. By controlling the oxidation peeling degree of CNTs, their interface area and defects are enhanced, thus producing more polarization centers to generate interfacial polarization and polarization relaxation, and also introducing more PANi loadings. Furthermore, more interface contact area can be produced between CNTs and PANi. This could induce a strong dielectric resonant and further improve the impedance matching, leading to significant enhancement of MA performance. With filler loading of only 10 wt % and a thinner coating thickness of 2.4 mm, the optimized CNTs@PANi exhibits excellent MA performance with the minimum reflection loss (RL) value of -45.7 dB at 12.0 GHz and the effective bandwidth is from 10.2 to 14.8 GHz. Meanwhile, the broadest effective bandwidth reaches 5.6 GHz, covering the range of 12.4-18.0 GHz with a thin thickness of 2.0 mm and its RL reaches -29.0 dB at 14.6 GHz. It is believed that the proposed interfacial modulation strategy can provide new opportunities for designing efficient MA absorbers.