Dual-layer thermal barrier coatings with ultra-high temperature resistance were prepared on the surface of molybdenum-rhenium alloy hot-end components. The preparation of the MoSi2- Gd2Zr2O7 dual-layer thermal barrier coatings was designed based on the coefficient of thermal expansion and coatings functionality and completed using atmospheric plasma spraying technology. The microstructure, mechanical properties, and thermal properties were analyzed. The results indicate that the adhesion of the prepared double-layer composite thermal barrier coatings is excellent, and no noticeable cracks appear at the interface. Compared to MoSi2 coatings with a low fracture toughness (0.88 MPa·m1/2), Gd2Zr2O7 coatings exhibits higher fracture toughness (1.74 MPa·m1/2) and stronger resistance to crack propagation. The prepared MoSi2- Gd2Zr2O7 composite coatings has a high porosity rate (39%), low thermal conductivity (1.02 W/m·K, 1200℃), and low thermal diffusivity (0.249 mm2/s, 1200℃). Additionally, it possesses a high oxygen vacancy concentration, resulting in a lower thermal diffusivity/thermal conductivity ratio, ensuring excellent insulation performance.