Piezoresistive fibers with large working factors remain of great interest for strain sensing applications involving large strains, yet difficult to achieve. Here, we produced strain-sensitive fibers with large working factors by dip-coating nanocomposite piezoresistive inks on surface-modified polyether block amide (PEBA) fibers. Surface modification of neat PEBA fibers was carried out with polydopamine (PDA) while nanocomposite conductive inks consisted of styrene–ethylene–butylene–styrene (SEBS) elastomer and carbon black (CB). As such, the deposition of piezoresistive coatings was enabled through nonconventional hydrogen-bonding interactions. The resultant fibers demonstrated well-defined piezoresistive linear relationships, which increased with CB filler loading in SEBS. In addition, gauge factors decreased with increasing CB mass fractions from ∼15 to ∼7. Furthermore, we used the fatigue theory to predict the endurance limit (Ce) of our fibers toward resistance signal stability. Such a piezoresistive performance allowed us to explore the application of our fibers as strain sensors for monitoring the movement of finger joints.