Despite the excellent physical properties of single-component Eu 3+-Tb 3+-containing metallopolymers, the development of their flexible WPLEDs for portable full-color flat displays remains a formidable challenge. Herein, we report the WPLEDs from a metallopolymer Poly(NVK-co-2-co-7), in which [Eu(DBM) 3 (4-vp-PBI)] (2) and [Tb(tba-PMP) 3 (4-vp-PBI)] (7) with different localized circumstances were grafted into PVK. In this design, both Dexter and Főrster energy transfers occurred, which endowed a photo-luminescent quantum yield up to 22.3% of the straightforward high-quality whitelights. Contributing from the stepwise alignment of frontier molecular orbitals of Poly(NVK-co-2-co-7) as the emitting layer in combination with CBP-and BCP-assisted carrier-transports, a reliable WPLED with the record-renewed electroluminescent performance (L Max = 388.0 cd/m 2 , c Max = 31.1 cd/A, p Max = 15.0 lm/W, EQE Max = 18.1% and weak efficiency-roll-off) among previous organo-Ln 3+based WOLEDs/WPLEDs was achieved. This finding renders single-component Eu 3+-Tb 3+-containing metallopolymers a potential new platform to cost-effective flexible WPLEDs for practical applications.