Recognizing the challenges of low strength, inadequate cementation, significant pore development, and excellent connectivity of reef limestone, as well as the persistent issues of ‘re-leakage’ and increasing leaks when using rigid bridge plugs, this paper posits the use of materials possessing both flexible and rigid properties for the prevention of leaks and plugging in reef limestone formations. Consequently, a plugging material exhibiting external flexibility and internal rigidity is developed (EFIR Material). This synergistic approach employs the deformability of flexible materials and the skeletal support of rigid materials to create a high-strength, dense plugging section. The new design enhances the formation’s pressure-bearing capacity while effectively addressing leakage issues. The material’s functional structure design, a core-shell structure of EFIR, is achieved by reverse-phase suspension polymerization of acrylamide (AM), 2-acrylamide-2-methylpropanesulfonic acid (AMPS), and alkyl ketone polymer (NVP), water-soluble monomers functioning as the shell and modified sand as the core. The results indicate that EFIR retains significant flexibility and strength upon water absorption and expansion. A sand bed made from 10 to 18 mesh calcareous sand exhibits excellent sealing properties. The optimal dosage of 3%-4% produces robust sealing effects, withstands pressures up to 7 MPa, and results in a tightly cemented, high-strength sand bed post-sealing with reef tuff, displaying high-quality sealing that is resistant to re-leakage.