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• The electron injection of ETL/perovskite of PeLEDs at molecular level is studied. • The molecular planarity bridging effects are discovered. • Superior molecular planarity of ETL enhances electron transport ability of ETL. • Superior molecular planarity of ETL improves carrier injection of ETL/perovskite. • Superior molecular planarity of ETL leads to superior performances of PeLEDs. Effectively balancing carrier injection of perovskite LEDs (PeLEDs) for next-generation display and illumination urgently needs for molecularly understanding carrier injection behavior of electron transport layer (ETL)/perovskite toward further developing high performance PeLEDs. Here, we molecularly reveal the electron injection behaviors of PeLEDs by theoretically-experimentally decoupling the electron transport of ETLs and electron injection of TmPyPB/perovskite and TPBi/perovskite. Resulted, the better molecular planarity bridging effect (MPBE) of TmPyPB than TPBi can effectively increase electronic-coupling for the improved electron transport ability and significantly decrease injection barrier for the enhanced electron injection capability, intrinsically leading to a more balanced carrier injection and a less electron accumulation of PeLEDs. Compared to TPBi-based PeLEDs, the TmPyPB-based PeLEDs present the obviously-increased average EQE, current efficiency, power efficiency and luminance by 44 %, 63 %, 43 % and 100 %, respectively. Meanwhile, this PeLED shows a higher voltage tolerance characteristic of 7.5 V than that of TPBi-based PeLEDs (6.25 V). Therefore, this work may provide a fundamental insight into carrier injection behavior of PeLEDs for effectively-regulating its carrier injection balance and further for its greatly-facilitated commercialization. [ABSTRACT FROM AUTHOR]