In this study, an improved CO2 separation and purification system is proposed based on in-depth analyses of cryogenic separation and distillation theory as well as the phase transition characteristics of gas mixtures containing CO2. Multi-stage compression, refrigeration, and separation are adopted to separate the majority of the CO2 from the gas mixture with relatively low energy penalty and high purity. Subsequently, the separated crude liquid CO2 is distilled under high pressure and near ambient temperature conditions so that low energy penalty purification is achieved. Simulation results indicate that the specific energy consumption for CO2 capture is only 0.425 MJ/kgCO2 with 99.9% CO2 purity for the product. Techno-economic analysis shows that the total plant investment is relatively low. Given its technical maturity and great potential in large-scale production, compared to conventional MEA and SelexolTM absorption methods, the cost of CO2 capture of the proposed system is reduced by 57.2% and 45.9%, respectively. The result of this study can serve as a novel approach to recovering CO2 from high CO2 concentration gas mixtures.