Optically clear pressure-sensitive adhesives (PSAs) face the challenges presented by a range of electronic and touch screen applications. Although many efforts have been made to manipulate the optical and adhesion properties of ultraviolet (UV)curable acrylate-based PSAs, further application and large-scale production are still limited owing to the intrinsically poor processability that stems from the large content of the high-vinylequivalent and low-viscosity acrylic monomers. Introducing a lowvinyl-equivalent and high-viscosity polyurethane acrylate (PUA) prepolymer into the formulation is a facile method to solve this issue without sacrificing the transparency. In this study, a series of PUA prepolymers are prepared to construct the model of PUA-co-2ethylhexyl acrylate (2EHA), denoted as poly(PUA-2EHA). The influence of PUA prepolymer architectures (average functionality and molecular features) on the optical and adhesion properties is elaborately discussed. The chemical cross-linking-induced enhancement of the haze values of PUA-based PSAs is investigated for the first time. Moreover, an improved and uniform bright image display without blemish, which is usually called the Mura defect-free image display in the industrial field, is obtained by using poly(PUA-2EHA) as the optically clear adhesive for full lamination of the thin-film transistor liquid crystal display (TFT-LCD) module. The laminated TFT-LCD module could be disassembled easily without leaving the residue on the screen. These results provide clear design guidelines to regulate the properties of PUA-based PSAs, which are especially valuable for the large-scale industrial production of UV-cured PSAs and facilitate the development of display technologies.