To develop CaO‐based sorbent pellets with highly efficient and stable CO2 capture capacity and sufficient mechanical strength for the application of calcium looping in circulating fluidized beds, Y2O3/MgO‐incorporated CaO‐based sorbents were fabricated via three synthesis methods and then sorbent pellets were prepared via extrusion and spheronization in the paper. Results showed that wet planetary ball milling was a good potential routine for large‐scale sorbent preparation. Additionally, impacts of liquid/solid ratio in wet ball milling and mass ratio of Y2O3/MgO were also investigated comprehensively. It was found that under the optimal liquid/solid ratio of 1:1 and Y2O3/MgO mass ratio of 2:1 determined, spherical Y2Mg1–1/1 sorbent exhibited desirable cyclic CO2 capture performance with a fast carbonation rate, achieving a CO2 uptake of 0.1399 g‐CO2/g‐sorbent after 62 cycles and improved about 31.1% in comparison of pure Ca (OH)2 pellets (CH). This was mainly owning to homogeneously distributed small grains and solid supports as well as enhanced pore structure in the wet ball‐milled pellets. Furthermore, long‐time fluidized attrition test was performed on the pellets, and the average attrition rate of Y2Mg1–1/1 was observed to be only one third that of CH. Even in the repeated carbonation/calcination process under high temperature, Y2Mg1–1/1 still possessed an excellent resistance to attrition.