The importance of energy storage increases where the potential of common technologies is expected to be not sufficient, in contrast to chemical energy storage (power-to-gas). In a power-to-gas context, electrical energy is used to produce hydrogen (H2), an energy carrier, via water electrolysis. This gas is required in several industries like refineries and the mobility sector (e.g. fuel cell hydrogen car). Nevertheless, the gas needs to be transported from production to consumers, especially when centrally produced at a large scale. For an energy- and cost-efficient distribution of a large amount of gas, pipelines are the best option. In the transition period to pure hydrogen networks, the co-transport in existing natural gas infrastructure is a particularly cost- and environmentally-efficient option. In previous work, a hybrid process based on membrane technology and pressure swing adsorption was designed to extract the transported hydrogen along the grid at fuel cell quality (99.97% (v/v) H-2 according to ISO 14687-2:2012). Further, the technical feasibility was demonstrated for the HylyPureprocess. In the current work, process simulation and optimisation was done to investigate different process designs in terms of their energy and process efficiency. The current work shows a developed process configuration that requires a significantly decreased total membrane area (reduction of 80%), a smaller PSA (size decrease of 50%) and is additionally about 60% more energy efficient. Furthermore, higher hydrogen recoveries are reachable with the new design. In a sensitivity analysis, the influence of various process parameters was investigated, identifying that the feed concentration, compression efficiency and particularly the process design have a major impact on the process performance. Simulations indicate that extracting hydrogen from a 4% (v/v) mixture with natural gas requires a specific energy demand of about 0.5-1.0 kWh m(-3) for hydrogen delivered at 25.81 bar.