Mechanically tough polymers with excellent room temperature self-healing capacity have aroused strong interest in soft electronics, electronic skins and flexible energy storage devices. However, achieving such polymers remains a challenge due to tardy diffusion dynamics. Herein, a robust and readily self-healing polymer, which is synthesized by one-pot polymerization among 2,4'-tolylene diisocyanate, isophorone diisocyanate, and poly(oxy-1,4-butanediyl), is achieved through reasonably tuning the hardness of the molecular segment and the strength of the dynamic crosslinking bond. The poly(oxy-1,4-butanediyl) that act as a soft segment can effectively avoid the microphase separation, enabling rapid chain mobility of the polymer at the room temperature. Furthermore, the dual H-bonding from 2,4'-tolylene diisocyanate segment acting as a relatively strong crosslinking bond contributes to high mechanical strength, while the weaker single H-bonding from isophorone diisocyanate segment can efficiently dissipate strain energy by bond rupture, endowing the polymer with rapid room temperature self-healing ability. Featuring state-of-the-art of robust stress strength (≈1.3 MPa), high self-healing efficiency (97% within 6 h), and large tensile strain (≈2100%), the resulting polymers are used for the fabrication of stretchable and self-healable electrical sensor, which can be employed to monitor a variety of physiological activities in real time. The described strategy is promising and universal for healable materials, displaying great potential for developing soft electronics. Copyright © 2019 Elsevier Inc. All rights reserved.