Despite as ignificant advancement in preparing metastable materials, one common problem is the strict and precious reaction conditions due to their metastable structures. Herein, we achieved the preparationo fh igh-temperature stabilized metastable a-MoC 1Àx by mounting zinc atoms into its lattice structure. Such as tructural construction could suppress the phase transformation from a-MoC 1Àx to b-Mo 2 C through restricting the displacement of Mo atoms upon increased temperature. The resultant metastable a-MoC 1Àx can be stabilized up to 1000 8Ca nd this stabilityt emperature is the highest for the metastable a-MoC 1Àx so far.S ynchrotron X-ray absorption spectroscopy (XAS) and X-ray photoelectron spectroscopy (XPS) confirm the structure of Zn-mount-ed a-MoC 1Àx .D ensityf unctional theory (DFT)c alculations revealt hat the introductiono ft he Zn atoms in the lattice structure of a-MoC 1Àx could significantly decrease the energy difference( DE)b etween a-MoC 1Àx and b-Mo 2 C, thus effectively suppressing the phase transformation from a-MoC 1Àx to b-Mo 2 Ca nd accordingly maintaining the hightemperature stability of a-MoC 1Àx .T his novel strategy can be used as au niversal methodt ob ee xtended to synthesize metastable a-MoC 1Àx from different precursors or other mounted elements. Moreover, the optimal product exhibits excellent lithium storage performances in terms of the cycling stability and rate performance. [c] P. Yang Chinese Academy of Engineering Physics Mianyang 621900 (P.R .China) Supporting information and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.Scheme1.The schematicillustration of the fabrication procedureofc ubic a-MoC 1Àx with high-temperature stability( yellow,black, and red balls, represent Mo, C, and Zn atoms, respectively).