It is of great significance to develop environmentally benign, non-volatile and recyclable green solvents for different applications. This feature article overviews the properties of green solvent systems (e.g., ionic liquids, supercritical carbon dioxide, deep eutectic solvents and mixed green solvent systems) and their applications in (1) framework material syntheses, including metal-organic frameworks, covalent organic frameworks and hydrogen-bonded organic frameworks, and (2) CO2 conversion reactions, including photocatalytic and electrocatalytic reduction reactions. Finally, the future perspective for research on green solvent systems is proposed from different aspects.