Flexible pressure sensor plays an important role in the field of human-computer interaction area due to its high flexibility and sensitivity. Convex surface of flexible electrodes provide an efficient way to enhance the sensitivity of flexible pressure sensors. However, facilely preparing controllable convex surface of flexible electrodes is still a challenge for obtaining high sensitive flexible pressure sensors. In this paper, direct-write print technique was utilized to prepare a concave structure surface with viscoelastic substrate, which could be used to prepare convex structure flexible electrode for fabricating highly sensitive flexible pressure sensors. Interaction between ink droplet and substrate was explored to generate a concave template, which could be controlled in spacing and diameter with printing spacing and nozzle diameter. Convex structure flexible surface could be prepared with the concave template, and then the convex structure flexible electrode could be realized with the evaporation of metallic silver on the surface. Furthermore, flexible pressure sensor was assembled with an interlocking structure by stacking two convex structure flexible electrodes in a face-to-face way, which could efficiently enhance flexibility and electrical property. The flexible pressure sensor presents a high sensitivity, a fast response/recovery time (<100 ms) and excellent flexibility (more than 10,000 cycles of bending), which could be applied in monitor physiological signals such as pulse detection, sound vibration, finger bending and so on. Therefore, this work provides an efficient method for preparing controllable structured surface, which has a great potential in the fabrication of flexible sensors, wearable electronics and energy devices.