Hyperbranched PEI and urea‐functionalized PEI amphiphiles are employed as additives in NBR compounding. Polarity design governing phase separation, PEI migration and PEI‐mediated self‐healing of NBR is demonstrated. The compatibility of PEI and NBR decreases with increasing molecular weight of PEI and with decreasing degree of substitution. Microphase‐separated NBR/PEI blends are prepared with varying PEI molecular architectures. Thermal self‐healing of NBR/PEI is monitored by applying tests combining crack initiation with annealing under compression. All PEI additives show complete crack‐healing upon annealing at 100 °C for 12 h. In contrast to neat NBR, the NBR/PEI‐2 blend afforded a self‐healing efficiency of 44% after cutting and re‐joining by compression and annealing.

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