High-strength nanocomposites were prepared by in situ polymerization of 2-methoxyethyl acrylate and N,N'-dimethylacrylamide with the existence of TiO2 nanoparticles. Based on the reversible hydrogen bond network, the resultant materials showed enhanced mechanical strength, excellent shape memory effect, and superior self-healing capability. To accomplish the goal of rapid and efficient self-healing for the materials, the elevated temperature was chosen as the healing temperature, and the fracture sample could be completely repaired within 10 min with the fracture strength of 13.56 MPa and high healing efficiency of similar to 100% (MD50-T5). Combining the high strain and water-absorbing nature of materials, the recovery of the complex shape of helix structure and self-lacing process in water under physiological temperature could be programmed and finished. Thus, the dual functional elastomers could be used in coating, suturing, and possess the wide application prospects in bioengineering and smart devices.