Multiple-phase nanocomposites filled with carbon nanotubes (CNTs) have been developed for their significant potential in microwave attenuation. The introduction of other phases onto the CNTs to achieve CNT-based heterostructures has been proposed to obtain absorbing materials with enhanced microwave absorption properties and broadband frequency due to their different loss mechanisms. The existence of polyaniline (PANI) as a coating with controllable electrical conductivity can lead to well-matched impedance. In this work, a one-dimensional CNT@BaTiO3@PANI heterostructure composite was fabricated. The fabrication processes involved coating of an acid-modified CNT with BaTiO3 (CNT@BaTiO3) through a sol–gel technique followed by combustion and the formation of CNT@BaTiO3@PANI nanohybrids by in situ polymerization of an aniline monomer in the presence of CNT@BaTiO3, using ammonium persulfate as an oxidant and HCl as a dopant. The as-synthesized CNT@BaTiO3@PANI composites with heterostructures were confirmed by various morphological and structural characterization techniques, as well as conductivity and microwave absorption properties. The measured electromagnetic parameters showed that the CNT@BaTiO3@PANI composites exhibited excellent microwave absorption properties. The minimum reflection loss of the CNT@BaTiO3@PANI composites with 20 wt % loadings in paraffin wax reached −28.9 dB (approximately 99.87% absorption) at 10.7 GHz with a thickness of 3 mm, and a frequency bandwidth less than −20 dB was achieved from 10 to 15 GHz. This work demonstrated that the CNT@BaTiO3@PANI heterostructure composite can be potentially useful in electromagnetic stealth materials, sensors, and electronic devices.

BaTiO₃@MWCNT heterostructures have been explored as microwave absorbers, which showed the maximum reflection loss with value of −25.7 dB at 12.1 GHz for 40 wt% loadings in wax, and the frequency bandwidth less than −20 dB is from 11.3 to 13.8 GHz.