Hybrid organic/inorganic perovskites are promising candidate materials for use in photovoltaic applications. More recently, they have also become highly attractive as active materials for other optoelectronic devices, including lasers, light-emitting diodes, and photodetectors. Nevertheless, difficulties in forming continuous and uniform films and the existence of a charge-injection barrier between the perovskite layer and the electrodes have hindered the development of high-performance perovskite light-emitting diodes (PeLEDs). In this study, a cross-linked hole-transport layer (HTL) is introduced to improve the hole-injection efficiency of PeLEDs. Furthermore, this layer simultaneously facilitates the formation of smooth perovskite layers, presumably because of the different surface energies. More interestingly, the HTL also exhibits strong solvent effects on the device performance. When the processing solvent for fabricating the HTLs is changed from chlorobenzene to N,N-dimethylformamide (DMF), the perovskite layer becomes more uniform and continuous, leading to better surface coverage and higher device efficiency, presumably because DMF has strong affinity toward the perovskite precursors. The approach presented herein could become a general method for decreasing the hole-injection barrier of PeLEDs and, eventually, lead to higher device performance.