Needle-like nanocrystalline mullite powders were prepared through the molten salt process at the temperature of 900 • C using coal gangue as raw material. Then, mullite-based composite ceramics were prepared by a conventional solid-state reaction between in situ synthesized mullite and Al 2 O 3 powders. Effects of Al 2 O 3 content and sintering temperatures on phase compositions, microstructure, and mechanical properties of the mullite-based composite ceramics were also studied. The results show that mullite content productivity increase from 72% to 95%, as the sintering temperature increased from 1480 • C to 1580 • C, which led to the improvement in the bulk density and flexural strength of the samples. The three-dimensional interlocking structure for mullite-based composite ceramics was obtained by the in situ solid-state reaction process. The maximum bulk density, flexural strength, and fracture toughness for the sample with 15 wt% Al 2 O 3 content are 2.48 g/cm 3 , 139.79 MPa, and 5.62 MPa⋅⋅m 1/2 , respectively, as it was sintered at the temperature of 1560 • C for 3 h. The improved mechanical properties of mullite-based composite ceramics maybe ascribed to good densification and increased mullite phase content, as well as to the in situ three-dimensional network structure. Therefore, the results would provide new ideas for high-value utilization of coal gangue.