Ruddlesden-Popper phase (RP-phase) perovskites that consist of 2D perovskite slabs interleaved with bulky organic ammonium (OA) are favorable for light-emitting diodes (LEDs). The critical limitation of LED applications is that the insulating OA arranged in a preferred orientation limits charge transport. Therefore, the ideal solution is to achieve a randomly connected structure that can improve charge transport without hampering the confinement of the electron-hole pair. Here, a structurally modulated RP-phase metal halide perovskite (MHP), (PEA)(2)(CH3NH3)(m-1)PbmBr3m+1 is introduced to make the randomly oriented RP-phase unit and ensure good connection between them by applying modified nanocrystal pinning, which leads to an increase in the efficiency of perovskite LEDs (PeLEDs). The randomly connected RP-phase MHP forces contact between inorganic layers and thereby yields efficient charge transport and radiative recombination. Combined with an optimal dimensionality, (PEA)(2)(CH3NH3)(2)Pb3Br10, the structurally modulated RP-phase MHP exhibits increased photoluminescence quantum efficiency, from 0.35% to 30.3%, and their PeLEDs show a 2,018 times higher current efficiency (20.18 cd A(-1)) than in the 2D PeLED (0.01 cd A(-1)) and 673 times than in the 3D PeLED (0.03 cd A(-1)) using the same film formation process. This approach provides insight on how to solve the limitation of RP-phase MHP for efficient PeLEDs.