The rapid decrease of CO2 capture capacity is one of the most challenging problems hindering the use of naturally occurring limestone in the calcium looping process. In this work, the mechanical modification method (dry planetary ball milling) was used to improve the cyclic CO2 capture performance of naturally occurring limestone. Low-cost Bayer aluminum hydroxide sourced from the industrial-scale production of alumina from bauxite ore was used as the precursor of the inert support to enhance the CO2 sorption stability of the ball-milled, sorbents. It was found that the CO2 uptake of the Milled sorbents could be further improved by increasing the ball-milling time because this generated more amounts of fine particles. Moreover, the pellets produced from ball-milled limestone powder possessed a relatively high. CO2 capture capacity of 0:252 g/g in the 25th cycle, which is nearly 1.3 times the capture capacity of naturally occurring limestone powder. This indicates that the combination of mechanical modification and pelletization is an effective approach to produce highly efficient CO2 capture pellets from naturally occurring limestone.