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The 2D C/C composites with different microstructures were fabricated by isothermal-isobaric chemical vapor infiltration (ICVI). The mechanical properties of the 2D C/C composites were investigated by 3-point bending tests. The microstructures of the pyrocarbon matrix were observed by polarized light microscope (PLM), scanning electron microscope (SEM), transmission electron microscope (TEM) combining selected area electron diffraction (SAED). The results show that 2D C/C composites with dominant layered-HT pyrocarbon matrix exhibit a pseudo-plastic failure behavior. The flake-like fragments MT and granular-like particles ISO are in favor of increasing the flexural strength of the materials. It exists a good interfacial bonding between the fiber and HT layer. The non-HT layer does not exist at the interface, but the orientation angle (OA) of the matrix slightly increases