The use of Pareto-optimal fronts to evaluate the full potential of reversible deactivation radical polymerization (RDRP) using multi-objective optimization (MOO) is illustrated for the first time. Pareto-optimal fronts are identified for activator regenerated electron transfer atom transfer radical polymerization (ARGET ATRP) of butyl methacrylate and nitroxide mediated polymerization (NMP) of styrene. All kinetic and diffusion parameters are literature based and a variety of optimization paths, such as temperature and fed-batch addition programs, are considered. It is shown that improvements in the control over the RDRP characteristics are possible beyond the capabilities of batch or isothermal RDRP conditions. Via these MOO-predicted non-classical polymerization procedures, a significant increase of the degree of microstructural control can be obtained with a limited penalty on the polymerization time; specifically, if a simultaneous variation of various polymerization conditions is considered. The improvements are explained based on the relative importance of the key reaction rates as a function of conversion.