Liquefaction of natural gas is an energy-intensive process in which the energy efficiency depends on the number of compressors stages and the heat integration scheme. The aim of the study is to systematically evaluate process performance of pure component cascade processes, present optimized designs for all relevant numbers of compression stages and compare energy consumption between processes with differing levels of complexity. An original method for the evaluation of process performance is developed that utilizes as little human interaction as possible, making it suitable for optimization. This study shows that a pure-component cascade process using the three refrigerants R290, R1150 and R50 must have at least 11 stages to equal the energy efficiency of the best mixed refrigerant process. An optimized configuration for an 11-stage process scheme operating at 20 ∘ C ambient temperature is described in detail.