Emulsion-based pressure-sensitive adhesives (PSAs) are gaining in importance due to their improved performance as well as the lower environmental impact of the emulsion polymerization process. In this study, the influence of eight emulsion polymerization variables on the final PSA properties of butyl acrylate/vinyl acetate (BA/VAc) emulsion-based PSAs was investigated (i.e., BA/VAc ratio, acrylic acid content, type and concentration of stabilizer, concentration of initiator, concentration of CTA, temperature, solids content). Final performance properties such as peel strength, shear strength, and tack were investigated on two different substrates: stainless steel and high-density polyethylene. A wide range of properties was generated ranging from very good to poor PSA performance. The screening design fulfilled its purpose in that it was used to generate a wide range of final properties. The results obtained here will be used in the decision-making process for further experimentation. However, for several reasons, the development of empirical models to relate the process conditions to the final product properties was not possible. In all three adhesive tests, the performance of the investigated adhesives was superior on the stainless steel substrate compared to high-density polyethylene. Most of the adhesives showed relatively high loop tack coupled with either adhesive or cohesive failure on both substrates. In most cases, peel strength was higher on stainless steel. A broad range of shear strength responses was observed: extremely high, on the order of several weeks, to zero shear strength. The chain transfer agent, which regulated the gel content of the emulsion latexes and the molecular weight of the soluble polymer fraction as well as the monomer feed composition, was suspected to be among the most influential factors affecting the final PSA performance. In addition, it was possible to obtain balanced final properties using either sodium dodecyl sulfate or poly(vinyl alcohol) as surfactant but at different concentrations.