AbstractAbrasion and tribological properties of tread rubber play a crucial role in governing the service life of aviation tires and the safety of aircrafts. Polyisoprene (IR) with the same chemical structure as natural rubber shows great potential for application in aviation tires. Herein, the abrasion and tribological behaviors of IR based composites under sliding‐rolling conditions were investigated in relation to the carbon black (CB N234) content, sliding‐rolling ratio, ambient temperature, and counterparts in order to provide guidance for the development of high‐performance aviation tire treads. Moreover, the relationship between wear performances and physical–mechanical properties was discussed to establish a prediction model. The results revealed that physical and mechanical properties affected wear performances in a synergetic manner, which could be described as a negative linear correlation of the folding wear with the product of hardness and rebound resilience (H4R) and the ratio between rebound resilience and tensile strength ((1‐R)/σ) even at elevated temperature and sliding‐rolling ratio regardless of the counterpart. The increase in CB N234 content and sliding‐rolling (s‐r) ratio resulted in a transition of the wear mechanism from folding to abrasion due to the formation of soft rubber particles with a certain fluidity and a lubricating transfer film that was located at the friction interface and was generated by the thermal‐mechanical degradation of the IR matrix when it was rubbed against steel counterparts, which marred the aforementioned negative linear relationship.Highlights The increase in temperature improved the abrasion resistance of tire treads. The folding wear was negatively and linearly related to H4R and (1‐R)/σ. Increasing CB N234 content and s‐r ratio made a transition of wear mechanism.