Acrylic pressure-sensitive adhesives (PSAs) were synthesized by solution polymerization using zirconium carboxyethyl acrylate (ZrCEA) with methyl aziridine derivatives (MAZ) as a curing agent. The acrylic PSAs were characterized by Fourier transform-infrared spectroscopy and gel contents. The viscoelastic properties of the acrylic PSAs were determined using an advanced rheometric expansion system. The adhesion performance of the acrylic PSAs was determined by measuring the probe tack, peel strength, shear adhesion failure temperature, and holding power. The optical properties of the acrylic PSAs were evaluated by the transmittance and refractive index. The results show that the adhesion performance and optical properties of the acrylic PSAs are influenced by the ZrCEA and MAZ content.