Flexible strain sensors are strongly demanded in fields of personal healthcare monitoring and human–machine interface, as they can accurately perceive external action to produce electrical output signals. Aiming at the existing problems, such as the balanced sensitivity and sensing range, durability as well as expanded application, this paper proposes a flexible strain sensor prepared based on electrospun thermoplastic polyurethane (TPU) membrane, followed by anchoring mixed conductive materials (carbon black (CB)/carbon nanotubes (CNT)) on its surface via an effective ultrasonic-assisted method. The resulting CB/CNT@TPU strain sensor delivers a desirable integration of sensing performances: good sensitivity, wide work range, fast response speed (<150 ms) and reliable cyclic stability (5000 cycles). Ascribed to the sensing behavior and additional breathability, strain sensor can be applied well to monitor human health, including human joints movements (fingers and wrists) and physiological signals (pulse and laryngeal vibration recognition). Finally, a multiaxial robotic arm control system is constructed, which provides a feasible strategy for intelligent robotic arms.