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A flexible, biocompatible, nitrile butadiene rubber (NBR)-based strain sensor with high stretchability, good sensitivity, and excellent repeatability is presented for the first time. Carbon black (CB) particles were embedded into an NBR matrix via a dissolving-coating technique, and the obtained NBR/CB composite was coated with polydopamine (PDA) to preserve the CB layer. The mechanical properties of the NBR films were found to be significantly improved with the addition of CB and PDA, and the produced composite films were noncytotoxic and highly biocompatible. Strain-sensing tests showed that the uncoated CB/NBR films possess a high sensing range (strain of ∼550%) and good sensitivity (gauge factor of 52.2), whereas the PDA/NBR/CB films show a somewhat reduced sensing range (strain of ∼180%) but significantly improved sensitivity (gauge factor of 346). The hysteresis curves obtained from cyclic …