Polycyclo-heteraborin multi-resonance (MR) emitters are promising for high color-purity organic light-emitting diodes (OLEDs). Here, unlike the most common heteroatom ternary-doped (X/B/N) frameworks, a binary-doped (B/N) skeleton is reported with a large energy band for wide-range color tunability. Based on this parent-segment, a "one-pot" catalyst-free borylation method is developed which generates deep blue to pure green MR emitters from readily available starting materials, with peaks at 426-532 nm and full-width-at-half-maxima of 27-38 nm. Impressively, a maximum external quantum efficiency of nearly 40 % is recorded for the corresponding device with Commission Internationale de l'Eclairage coordinates of (0.14, 0.16), representing the state-of-the-art performances. This work presents a new paradigm and synthesis of B/N-doped MR emitters and will motivate the study of other novel frameworks.
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