One of the most challenging tasks in fabricating multilayer polymer light-emitting diodes (PLEDs) by solution processes is to avoid the interfacial mixing between different layers because most of the commercially available emissive and charge-transporting materials are soluble in common organic solvents. To overcome this difficulty, extensive efforts have been invested in developing novel crosslinkable hole-transporting materials (HTMs). After thermo- or photo-crosslinking, all these crosslinked HTMs possess very good solvent resistance which greatly facilitates the subsequent processing of the emitting layer. By taking advantage of these HTMs, high efficiency red-green-blue (RGB)-emitting PLEDs, as well as white- and quantum dot based PLEDs, have been realized. This article provides a brief overview of the recent development of crosslinkable HTMs and their unique advantages in enhancing the performance of LEDs.