A method of using modified epoxy resin (PEG‐E51) and graphene oxide (GO) as sizing agent in different pH has been proposed and applied to improve the interfacial interactions and bonding of carbon fiber (CF) reinforced epoxy resin‐based (EP) composites. The PEG‐E51 and GO complex sizing in different pH is prepared and then coated on CF surfaces homogeneously. The sizing layer forms on the fiber surfaces, and multiple GO sheets are introduced successfully surrounding the CFs. The surface morphologies of CFs change distinctly with different pH. The interfacial shear strength increases from 51.36 MPa for bare fiber‐reinforced EP composites to 66.62 MPa for composites reinforced by CFs coated with GO only. However, a significant improvement is achieved when the pH is adjusted to 10, making the interfacial shear strength grow up to 77.23 MPa. Furthermore, scanning electron microscopy results and interlaminar shear strength test are in agreement with each other, suggesting better interface bonding of composites by regulating pH of PEG‐E51 and GO complex sizing. Besides, the interfacial interaction mechanism in CF reinforced composites is also explored, that is, the positive effects of roughness and specific surface area in complex interfacial layers lead to the improvement of interfacial properties.

Based on the strategy of killing two birds with one stone, we introduce thermally expandable microspheres into a silicone rubber matrix to fabricate temperature-responsive controllable deformation materials, which exhibit intelligent deformation properties as well as enhanced thermal protection performance, for dynamic thermal protection in the next-generation morphing aircrafts. The formation of hollow structures endows the material with intelligent thermal management ability and makes the thermal conductivity controllable, meeting the requirements of rapid deformation and excellent thermal insulation. The dimensions of the material adaptively expand with increasing temperature, and a constant 50N force can be provided to ensure reliable sealing. Moreover, benefiting from the synergistic effect of the hollow structure and zinc borate in the ceramization process of the silicone rubber, the 10 mm thick material can reduce the temperature from 2000 to 63 °C, and the mass ablation rate is only 4.8 mg/s. To broaden the application of our material, a sensor with a sandwich structure composed of different functional layers is designed. It is pleasantly surprising to observe that the sensor can provide real-time remote warning of fire and overheating sites with a response time as short as 1 s. This synergistic strategy opens a new possibility to fabricate intelligent thermal protection materials.