In this study, exfoliated montmorillonite (MMT) nanolayers were successfully encapsulated in acrylamide/acrylic acid/2acrylamido-2-methylpropanesulfonic acid (AM/AA/AMPS) terpolymer microspheres by in situ inverse suspension polymerization with the aid of the organic intercalation modification and the lateral groups of terpolymer chains. The introduction of well-dispersed MMT nanolayers reveals a significant enhancement of the comprehensive properties of these nanocomposite microspheres, such as the viscoelasticity, thermal stability, and plugging ability. Compared with the pure terpolymer, the elastic modulus (G 0 ) of terpolymer/2.0 wt % O-MMT nanocomposites is 4.30 times higher and the decomposition temperature of these nanocomposites increases by 40 8C. The plugging rate reaches as high as 86.6%. Besides, surface morphology, swelling degree, and wetting behavior can be effectively tuned by varying the content of exfoliated MMT. The wetting angle increases to 82.0 8 which is suitable for modifying the formation channels. These selected nanocomposite microspheres can effectively enter and plug the high permeable microchannels.Polymer nanocomposites containing inorganic nanoparticles are gathering increasing attention owing to their remarkable improvements in mechanical and thermal properties compared with pristine polymer. 5,6 Montmorillonite (MMT) is one of the most widely used inorganic layered silicates because the lamellar elements exhibit high in-plane strength, stiffness, and a high aspect ratio. 7,8 Strong interfacial interactions between the dispersed layers and the polymer matrix can significantly enhance the mechanical, thermal and barrier properties of the virgin polymer. 9 Moreover, the dispersed MMT layers can also exhibit catalytic, nucleation, and crosslinking effects that adjust the morphology and function of the polymers. [10][11][12] The properties of the obtained polymer/ MMT nanocomposites depend on the level of MMT platelet delamination and the MMT dispersion in the polymer matrices. 13 Well-dispersed MMT layers, especially exfoliated layers, cannot be easily achieved due to their preference for face-to-face stacking in agglomerated tactoids during polymerization. 14,15 Presently, some