Model acrylic pressure-sensitive adhesives (PSAs) based on poly(2-ethyl-hexyl acrylate-stat-acrylic acid) and poly(n-butyl acrylate-stat-acrylic acid) at 97.5/2.5 wt % were synthesized using semicontinuous emulsion and solution polymerizations. Microgels formed in the lattices retained their discrete network morphology in the film. In contrast, acrylic solution was essentially gel free and crosslinking in the film was provided by the reaction of acrylic acid and post added Al Acetyl Acetonate after solvent evaporation, which led to continuous network morphology. The difference in film network morphology caused significantly lower shear holding power for the film from emulsion PSA compared with that of solvent-borne film. Unlike shear holding power, loop tack and peel of acrylic PSAs were mainly controlled by the same sol/gel molecular parameters, regardless of emulsion or solution PSAs. The important molecular parameters are sol-to-gel ratio, entanglement molecular weight, weight average molecular weight, and to a lesser extent, glass transition temperature.