Efficient perovskite light-emitting diodes are designed by employing an ordered vertical domain distribution in quasi-two-dimensional (quasi-2D) perovskites to induce better electron flow to the emitting domains. Dimethyl sulfoxide is added to the precursor solution to tune the crystallization rate and promote the formation of high-m domains near the substrate surface via the one-step deposition method. Optimized deposition conditions yielding a film with favorable energetic landscape for both carrier injection and confinement results in a 4-fold external quantum efficiency (EQE) enhancement with maximum EQE of 5.79%. Better carrier injection is further supported by a turn-on voltage value that is comparable to the band gap of the emitter material (∼2.25 eV).