Introducing spiral polycyclic aromatic hydrocarbons (PAHs) in multiple resonances thermally activated delayed fluorescence (MR-TADF) emitters to achieve small FWHM values and high efficiency remains a formidable challenge. This research departs from the conventional molecular design strategy that utilizes spiral PAHs solely as side chains, terminal groups, or linkage units. Instead, we integrate the rigid 9,9'-spirobi[fluorene] (SF) unit fully or partially into the boron/ nitrogen MR (B/N-MR) emitting core and successfully developed a range of brand-new proof-of-concept isomerized MR-TADF emitters, SF-BN1, SF-BN2, SF-BN3, and SF-BN4. Remarkably, these novel emitters exhibit exceptionally narrow full-width at half-maximum (FWHM) values of 15~21 nm in dilute toluene solutions and high photoluminescence quantum yields (PLQYs) of up to 90% in doped films. The corresponding organic light-emitting diode (OLED) based on SF-BN1 achieved high external quantum efficiency (EQE) of up to 29.0%, with CIE coordinates of (0.13, 0.08), closely aligning with the BT.2020 blue emission standard. Sky-blue OLEDs based on SF-BN3 can achieve a high EQE of 29.8%, with an exceptionally highly narrow FWHM value of 18 nm; the hyperfluorescent OLEDs based on SF-BN3 improved the EQE of 35.5%. Moreover, we elucidated subtlevariations in the connectivity of chemical functional groups within emitters, as well as the polar environment and doping concentrations of OLEDs, which can significantly impact the optical and electroluminescent properties of these isomers. This research unveils new opportunities for exploration and yields potential novel luminescent materials suitable for ultra-high-definition (UHD) display technologies.