The traditional methods for preparing magnesium aluminum layered double hydrotalcite (Mg2Al-CO3LDHs) in industry include coprecipitation and hydrothermal methods. Both these methods have the disadvantages of high preparation cost and complicated water washing process. Using Mg(OH)2, Al(OH)3, and CO2 as raw materials in this work, the Mg2Al-CO3 LDHs are successfully prepared by mechanochemical method, which solves the shortcomings of traditional preparation method and realizes the conversion and utilization of CO2 resource. The prepared Mg2Al-CO3 LDHs are evaluated as a heat stabilizer in poly(vinyl chloride) (PVC). The result indicates that, when 2.4 phr Mg2Al-CO3 LDHs, 0.3 phr ZnSt2, and 0.3 phr of zinc acetylacetonate are added to the PVC, the thermal stability time of PVC can reach 190 min, which is better than PVC containing commercial Mg2Al-CO3 LDHs. Meanwhile, its processing performance is basically the same as the PVC containing commercial Mg2Al-CO3 LDHs.