Cross-linking network structures are critical to construct flexible and lightweight electromagnetic (EM) wave absorbers, for which effective regulation of the EM parameters is essential. Herein, a versatile strategy has been developed by interconnecting carbon fibers with NiFe-layered double hydroxide (NiFe LDH)/MXene derivatives. The large-sized flaky morphology and conductive nature of the interconnectors induce the percolation effect in the fabric networks with ultralow addition. As such, efficient adjustment of the EM parameters can be achieved by tuning the content of the interconnectors around the percolation threshold, giving rise to an optimal reflection loss (RL) of -58.0 dB and a wide effective absorption band (EAB) of 7.0 GHz at a thickness of 2.5 mm under the incorporation of 7.0 wt % NiFe LDH/MXene. This work provides insights on constructing percolation networks and effective manipulation of electronic and magnetic properties, which can be extended to various areas such as sensing, catalysis, and energy storage.