The integration of multi-dimensional materials is a powerful approach for the construction of high-performance microwave absorbers. In this work, 2D-like carbon microsheets (CMSs) have been directly synthesized on the surfaces of 3D helical carbon nanocoils (CNCs) through a Cu catalyzed chemical vapor deposition process. The junctions formed between CMSs and CNCs create numerous polarization sites, which enhances interfacial polarization. The planar morphology of CMSs is beneficial to enhance the multiple scattering of microwave, while the 3D helical CNCs prevent the aggregation of 2D-like CMSs and simultaneously enhance the conductive loss and cross-polarization loss. By controlling the growth time, the morphologies of CMS are precisely tailored and their impedance matching is adjusted. Consequently, CMS/CNC demonstrates exceptional microwave absorption (MA) performance with a broad effective bandwidth of 6.5 GHz and a minimum reflection loss of −39.3 dB at a remarkably low filling ratio of 4 wt%. This study provides a novel multi-dimensional integrated structure for efficient MA.