Metallic 1T phase of MoS2 (1T-MoS2) has aroused great concern for decontamination of heavy metal ions from water. Herein, ultrastable 1T-MoS2 was successfully achieved via a gentle two-stage solvothermal strategy utilizing water and ethanol as solvent for efficient removal of Cr(VI). Notably, nearly 100 % 1T-MoS2 was obtained, and it remained highly stable in air even for 360 days. Electron paramagnetic resonance analysis showed that sulfur vacancies were in situ formed on the 1T/2H mixed phase MoS2 (M-MoS2) under the induction of ethanol, which is critical to promote the transformation of 2H to 1T phase. Molecular dynamic simulation revealed that there was strong interaction between ethanol and MoS2 surface, which could decrease the total energy of MoS2 for strengthening stability of 1T phase. Moreover, 1T-MoS2 shows superior sorption capacity (200.3 mg·g−1) for removal of Cr(VI), twice more than that of M-MoS2 and 2H phase MoS2 under the same condition. Significantly, the stable phase structure of 1T-MoS2 and chromium adsorption capacity still remained even after five cycles of chromium adsorption. The study of Cr(VI) adsorption mechanism revealed that the chromium adsorption was attributed to the undercoordinated Mo(IV) as active site and coupled with redox reaction during removal process.