This dissertation concerns the development of simulation and optimization technology for industrial, hydrolytic nylon-6 polymerizations. The significance of this work is that it is a comprehensive and fundamental analysis of nearly all of the pertinent aspects of simulation. It steps through all of the major steps for developing process models, including simulation of the reaction kinetics, phase equilibrium, physical properties, and mass-transfer- limited devolatization. Using this work, we can build accurate models for all major processing equipment involved in nylon-6 production. Contributions in this dissertation are of two types. Type one concerns the formalization of existing knowledge of nylon-6 polymerization mixtures, mainly for documentation and teaching purposes. Type two, on the other hand, concerns original research contributions. Formalizations of existing knowledge include reaction kinetics and physical properties. Original research contributions include models for phase equilibrium, diffusivities of water and caprolactam, and devolatization in vacuum-finishing reactors. We have designed all of the models herein to be fundamental, yet accessible to the practicing engineer. All of the analysis was done using commercial software packages offered by Aspen Technology, Cambridge, MA. We chose these packages for two reasons: (1) These packages enable one to quickly build fundamental steady-state and dynamic models of polymer trains; and (2) These packages are the only ones commercially available for simulating polymer trains. / Ph. D.