Solution-processable organometal halide perovskites have been emerging as very promising materials for light-emitting diodes (LEDs) because of their high color purity, low cost, and high photoluminescence quantum yield. However, their electroluminescent performance is still limited by incomplete surface coverage and inefficient charge injection into the perovskite. Here, we demonstrate highly efficient perovskite LEDs (PeLEDs) incorporating full film coverage and bipolar charge injection within the active layer by introducing perovskite precursor poly(9-vinylcarbazole):1,3,5-tris(1-phenyl-1H-benzimidazol-2-yl)benzene (PVK:TPBi) toluene solution into CH3NH3PbBr3 N,N-dimethylformamide solution. Both the film coverage and the charge injections were simultaneously improved by antisolvent of toluene and PVK:TPBi matrix, respectively. After the film morphology and weight ratio of PVK:TPBi were carefully adjusted, the optimal PeLEDs gave efficient emission with turn-on voltage of ∼2.8 V, maximum luminance of ∼7263 cd/m2, maximum current efficiency of ∼9.45 cd/A, and maximum external quantum efficiency of ∼2.28%, which are among the best results based on MAPbBr3 reported to date.