Perovskite light-emitting diodes (PeLEDs) are considered as promising candidates for next-generation solution-processed full-color displays. However, the external quantum efficiencies (EQEs) and operational stabilities of deep-blue (<460 nm) PeLEDs still lag far behind their red and green counterparts. Herein, a rapid crystallization method based on hot-antisolvent bathing is proposed for realization of deep-blue PeLEDs. By promoting immediate removal of the precursor solvent from the wet perovskite films, development of the quasi-two-dimensional (2D) Ruddlesden–Popper perovskite (2D-RPP) crystals with n values >3 is hampered completely, so that phase-pure 2D-RPP films with bandgaps suitable for deep-blue PeLEDs can be obtained successfully. The uniquely developed rapid crystallization method also enables formation of randomly oriented 2D-RPP crystals, thereby improving the transfer and transport kinetics of the charge carriers. Thus, high-performance deep-blue PeLEDs emitting at 437 nm with a peak EQE of 0.63% are successfully demonstrated. The color coordinates are confirmed to be (0.165, 0.044), which match well with the Rec.2020 standard blue gamut and have excellent spectral stability.