In this study, sodium carboxymethyl cellulose/poly(acrylic acid) (CMC/PAA) microgels were successfully synthesized via visible-light-triggered free-radical polymerization to remove methylene blue (MB) from water. The microgels had a loose and porous 3-D network structure, exhibiting excellent adsorption performance. The equilibrium adsorption capacity and the removal efficiency of the microgels reached approximately 1479 mg/g and 97%, respectively, when the initial concentration of MB was 300 mg/L. The adsorption kinetics was well described by the pseudo-second-order model, and the adsorption isotherms followed the Langmuir isothermal model. Notably, CMC/PAA microgels could naturally settle and be separated from the MB solution. Furthermore, the recovery efficiency of the regenerated CMC/PAA microgels reached approximately 94% after five adsorption-desorption cycles. Therefore, the microgels could be used as promising adsorbents due to the advantages of high adsorption capacity, fast removal rate, and reusability.