Flexible piezoelectric PZT/fabric composite material is pliable and tough in nature which is in a lack of traditional PZT patches. It has great application prospect in improving the sensitivity of sensor/actuator made by piezoelectric materials especially when they are used for curved surfaces or complicated conditions. In this paper, glass fiber cloth was adopted as carrier to grow PZT piezoelectric crystal particles by hydrothermal method, and the optimum conditions were studied. The results showed that the soft glass fiber cloth was an ideal kind of carrier. A large number of cubic‐shaped PZT nanocrystallines grew firmly in the carrier with a dense and uniform distribution. The best hydrothermal condition was found to be pH 13, reaction time 24 h, and reaction temperature 200°C.