The (00h) BaFe12O19 (BaM) filled Co2Y@PANI composite with oriented microstructure have been prepared by an in-situ polymerization reaction and a tape-casting method. Firstly, the hexaferrite Ba2CO2Fe12O22 (Co2Y) nanoparticles was modified and coated by polyaniline (PANI) to form a Co2Y@PANI core-shell composite. Then the Co2Y@PANI composite with 10 wt% (00h) BaFe12O19 tempaltes were mixed in Polyvinyl Butyral (PVB) matrix and finally formed the Co2Y@PANI/BaM-T/PVB composite sheet via the tape-casting process. Under the shear forces during the tap-casting, the BaM templates were orderly dispersed in the composite to form an oriented microstructure to enhance the scattering effect. Furthermore, the microwave absorption ability of Co2Y, Co2Y@PANI and Co2Y@PANI/BaM-T in PVB matrix were investigated from 2 to 18 GHz frequency. The maximum reflection loss value of Co2Y@PANI/BaM-T/PVB composite can reach -66.9 dB at 11.6 GHz with 1.9 mm thin thickness and broad effective bandwidth (RL < -10 dB) about 6.32 GHz. The excellent EMA properties were ascribed to the high performance dielectric-magnetic hierarchical architectures. This work demonstrates the great potential of the structural design utilizing ferrite materials for microwave absorbing application.