The cost of currently available technologies for CO2 capture should be further reduced to allow for large scale implementation of Carbon Capture and Storage. Solvents for CO2 capture systems with physical absorption are usually selected based on heuristics, engineering expertise and experimental trials. The performance of the separation system is, however, defined by both the properties of the selected solvent and the process conditions, which should be considered simultaneously. In this thesis, the Continuous Molecular Targeting - Computer Aided Molecular Design (CoMT-CAMD) framework is extended and applied to the simultaneous optimization of process and solvent for CO2 capture systems with physical absorption.@en