A one-pot, two-step miniemulsion polymerization approach was successfully used to create poly(2-ethyl hexyl acrylate/methyl methacrylate/acrylic acid) pressure sensitive adhesives with well-defined and predictable bimodal particle size distributions (PSDs) or bimodal molecular weight distributions (MWDs). The resulting viscoelastic (shear storage and loss moduli) and adhesive properties (i.e., loop tack, peel strength, and shear strength) were tested and compared to monomodal distributions of either particle size or molecular weight along with bimodal distributions created by postpolymerization blending. The results indicated that in situ bimodal MWDs offered superior values of PSA properties when compared to either monomodal MWDs or postpolymerization blends. Viscoelastic analysis of the in situ bimodal MWD samples showed that the proposed approach can effectively vary the MWDs and cross-linking densities of the resulting PSAs, thus tailoring the final properties. In comparison, the in situ bimodal PSD latexes did not show significant differences in viscoelastic behavior, but they exhibited large differences in PSA properties.