Multiple resonance (MR) compounds have garnered substantial attention for their prospective utility in wide color gamut displays. Nevertheless, developing red MR emitters with both high efficiency and saturated emission color remains demanding. We herein introduce a comprehensive strategy for spectral tuning in the red region by simultaneously regulating the π-conjugation and electron-donating strengths of a double boron–embedded MR skeleton while preserving narrowband characteristics. The proof-of-concept materials manifested emissions from orange-red to deep red, with bandwidths below 0.12 eV. The pure-red device based on CzIDBNO displayed superior color purity with CIE coordinates of (0.701, 0.298), approaching the Broadcast Television 2020 standard. In concert with high photoluminescence quantum yield and strong horizontal dipole orientation, CzIDBNO also achieved a maximum external quantum efficiency of 32.5% and a current efficiency of 20.2 cd A
−1
, outstripping prior reported organic light-emitting diodes (OLEDs) with CIE
x
exceeding 0.68. These findings offer a roadmap for designing high-performance emitters with exceptional color purity for future OLED material research advancements.