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The affecting mechanism of activation conditions on the performance of NaNO3-modified dolomites for CO2 capture was conducted combined with the activation tests and the CO2 absorption tests. The weight loss during activation was determined by the combined effects of the NaNO3 content, activation temperature, and activation atmosphere, for their combined effects on the ion diffusion. Moreover, the greater weight loss during activation did not elicit a corresponding increase in CO2 absorption ability of the activated absorbents. CO2 absorption activity tests indicated that the sample 0.20Na-dol activated at 500 °C in N2 showed the best cyclic CO2 absorption ability. The underlying mechanism was then analyzed based on the results of the Brunauer-Emmett-Teller, X-ray diffraction, and Raman analysis of the absorbents. The results indicated that the different CO2 absorption abilities might be due to the two kinds of molecular arrangements between the MgO and CaCO3 grains obtained during activation. © 2015 Curtin University of Technology and John Wiley & Sons, Ltd. [ABSTRACT FROM AUTHOR]