A demethaniser process is characterised by interactions between the complex distillation column and other flowsheet units, including the turbo-expander, flash units, multistream exchangers and refrigeration system. When a design problem dealing with demethaniser flowsheets is approached in a systematic way, the number of alternatives to be studied is generally very large. The assessment of all possible flowsheets with numerous options is a time consuming task with many simulations required to select the most economic option. This research presents a systematic approach for demethaniser flowsheet synthesis to generate cost-effective designs with minimal time and effort. A demethaniser column has many degrees of freedom, including the operating pressure, multiple feeds, the number and duty of side reboilers and the flow rate of the external reflux stream. The additional feed and side reboiler streams enhance the efficiency of the process, but complicate process modelling. The number of design variables is also augmented by additional degrees of freedom such as the location and the order of feeds, the number of stages and the reflux ratio in the column. The complexity of the demethaniser column precludes the use of the Fenske-Underwood-Gilliland shortcut design method. A semi-rigorous boundary value method is proposed for the design of complex demethaniser columns for application within an optimisation framework for process synthesis and evaluation. The results of the proposed design methodology are shown to be in good agreement with those of rigorous simulation.A simplified flowsheet simulation model based on a sequential modular approach is developed that is able to account for various configurations and inter-connections in the demethaniser process. Improved shortcut models for flash units, the turbo-expander, compressor and refrigeration cycle have been proposed for exploitation in a synthesis framework. A methodology accounting for heat integration in multistream exchangers is proposed. The simplified simulation model is applied for the optimisation of a flowsheet of fixed configuration. The nonlinear programming technique of sequential quadratic programming (SQP) is used as the optimisation method. A case study is presented to illustrate the application of the optimisation approach for maximising the annual profit.A generalised superstructure has been proposed for demethaniser flowsheet synthesis that includes various structural combinations in addition to the operational parameters. The various options included in the superstructure and their effects on flowsheet performance are discussed. A stochastic optimisation technique, simulated annealing, is applied to optimise the superstructure and generate energy-efficient and cost-effective flowsheets. The application of the developed synthesis methodology is illustrated by a case study of relevance to natural gas processing. The results allow insights to be obtained into the important trade-offs and interactions and indicate that the synthesis methodology can be employed as a tool for quantitative evaluation of preliminary designs as well as to facilitate evaluation, selection and optimisation of licensed demethaniser flowsheets.