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[Display omitted] Core-shell structure has been receiving extensive attention to enhance the electromagnetic wave (EMW) absorption performance due to its unique interface effect. In this paper, a micro-flower like ZnCo@C@1T-2H-MoS 2 was prepared through MOF self-template method. The introduction 1T-2H-MoS 2 shell helps optimize impedance matching of the CoZn@C particles to improve the EMW absorption ability. The minimal reflection loss (RL min) value of ZnCo@C@1T-2H-MoS 2 is −35.83 dB with a thickness of 5.0 mm at 5.83 GHz and the effective absorption (RL < -10 dB) bandwidth up to 4.56 GHz at 2.0 mm thickness. Meanwhile, the overall effective absorption bandwidth (OEAB) can reach up to 13.44 GHz from 4.56 to 18.0 GHz. Moreover, ultrafast photothermal performances are also achieved, which can guarantee the normal functioning of ZnCo@C@1T-2H-MoS 2 materials in cold conditions. The excellent EMW absorption and photothermal performance are attributed to the unique structure designed with the core of magnetic ZnCo@C rhombic dodecahedral and the shell of dielectric micro-flower like 1T-2H-MoS 2 optimize impedance matching. [ABSTRACT FROM AUTHOR]