CO2 absorption/release properties of limestone mixed with 2.5∼40 mass% reagent grade-SiO2 powders or natural diatomite have been investigated. XRD analysis of calcined diatomite-mixed limestone revealed the formation of Ca2SiO4. However, only CaO and SiO2 were confirmed in the case of the calcined limestone mixed with reagent grade-SiO2 powders. Addition of reagent grade-SiO2 and natural diatomite led to improvement of CO2 absorption capacity of limestone ore. In the initial absorption process, limestone mixed with 10 mass% reagent grade-SiO2 showed the highest degree of absorption (67%; 673 K, 21.6 ks). In the case of natural diatomite, CO2 absorption degree attained maximum (∼55%) at 5 mass% of natural diatomite. Furthermore, the absorption durability of limestone ore was improved by the addition of reagent grade-SiO2 or natural diatomite. These results indicate that the addition of reagent grade-SiO2 particles or natural diatomite is an efficient way to improve the absorption properties of natural limestone ore.