In situ CO2 mixing technology is a potential technology for permanently sequestering CO2 during concrete manufacturing processes. Although it has been approved as a promising carbon capture and utilisation (CCU) method, its effect on the leachability of heavy metals from cementitious compounds has not yet been studied. This study focuses on the effect of in situ CO2 mixing of cement paste on the leaching of hexavalent chromium (Cr(VI)). The tank leaching test of the CO2 mixing cement specimen resulted in a Cr(VI) cumulative leaching of 0.614 mg/m2 in 28 d, which is ten times lower than that of the control mixing specimens. The results in thermogravimetric analysis indicated that a relatively significant amount of CrO42− is immobilised as CaCrO4 during the CO2-mixing, and a higher Cr–O extension is observed in the Fourier transform infrared spectra. Furthermore, a portion of the monocarboaluminate is inferred from microstructural analyses to incorporate CrO42− ions. These results demonstrate that in situ CO2 mixing is beneficial not only in reducing CO2 emissions, but also in controlling the leaching of toxic substances.