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Hybridized local and charge‐transfer (HLCT) with the utilization of both singlet and triplet excitons through the "hot excitons" channel have great application potential in highly efficient blue organic light‐emitting diodes (OLEDs). The proportion of charge‐transfer (CT) and locally excited (LE) components in the relevant singlet and triplet states makes a big difference for the high‐lying reverse intersystem crossing process. Herein, three novel donor (D)‐acceptor (A) type HLCT materials, 7‐([1,1′‐biphenyl]‐4‐yl(9,9‐dimethyl‐9H‐fluoren‐2‐yl)amino)‐3‐phenyl‐1H‐isochromen‐1‐one (pPh‐7P), 7‐([1,1′‐biphenyl]‐4‐yl(9,9‐dimethyl‐9H‐fluoren‐2‐yl)amino)‐3‐methyl‐1H‐isochromen‐1‐one (pPh‐7M), and 6‐([1,1′‐biphenyl]‐4‐yl(9,9‐dimethyl‐9H‐fluoren‐2‐yl)amino)‐3‐methyl‐1H‐isochromen‐1‐one (pPh‐6M), were rationally designed and synthesized with diphenylamine derivative as donor and oxygen heterocyclic coumarin moiety as acceptors. The proportions of CT and LE components were fine controlled by changing the connection site of diphenylamine derivative at C6/C7‐position and the substituent at C3‐position of coumarin moiety. The HLCT characteristics of pPh‐7P, pPh‐7M, and pPh‐6M were systematically demonstrated through photophysical properties and density functional theory calculations. The solution‐processed doped OLEDs based on pPh‐6M exhibited deep‐blue electroluminescence with the maximum emission wavelength of 446 nm, maximum luminance of 8755 cd m−2, maximum current efficiency of 5.83 cd A−1, and maximum external quantum efficiency of 6.54 %. The results reveal that pPh‐6M with dominant 1LE and 3CT components has better OLED performance. [ABSTRACT FROM AUTHOR]