Glass fiber reinforced polytetrafluoroethylene composites (PTFE/GF composites) with the excellent performance have been given considerable attention due to their increasing applications in large architecture areas such as stadiums, amusement parks, parking lots, etc. However, the brittleness of glass fiber can hinder the performance of PTFE/GF composites. The PTFE/MLDH (modified ZnAl‐layered double hydroxide)/GF composites inspired by layer‐layer structure are prepared via the multi‐layered dipping method, which consists of GF acting as a reinforcement, PTFE acting as matrix, and MLDH acting as the layer‐layer structure. The results of study show that the high strength and surperflexibility of PTFE/MLDH/GF composites are higher than pure PTFE/GF composites. Especially, when the PTFE/MLDH/GF composites contain 1.6 wt% MLDH, the folding endurance reaches up to 39 035 times, the tensile strength reaches up to 163.57 MPa, and strain reaches up to 8.33%. More significantly, the strength and surperflexibility are illustrated by a mechanism model and it is used to further broaden the application of PTFE/GF composites in mobile building materials. Moreover, it is discovered that the PTFE/MLDH/GF composites have unique translucent performance and excellent ultraviolet‐shielding properties in this study, which further broaden its range of applications.