Metal–organic frameworks (MOFs) are promising candidates for CO2 capture and conversion as they possess remarkable properties, including large surface area, open channels and permanent porosity. Through the judicious selection of metal clusters and organic linkers, a framework with a desired topology can be realized. Furthermore, the study of the noncovalent interactions in MOFs provides significant insights into the relationship between the catalytic performance and the framework structure, which will also further promote the development of MOFs as heterogeneous catalysts for CO2 capture and conversion. This chapter is divided into four sections. The first section gives a brief introduction to the structures and chemical features of MOFs. The second section concentrates on MOFs as heterogeneous catalysts for the chemical fixation of CO2 with organic compounds. The third section presents MOFs as photocatalysts for CO2 reduction. The last section covers the application of MOFs in the electrocatalytic reduction of CO2. Particular challenges in the rational design and application of MOF catalysts and research opportunities for further development are highlighted. It is hoped that this chapter will not only serve as a starting point to gain insights into this challenging field but will also stimulate more intensive research on the development of creative MOFs as heterogeneous catalysts towards CO2 capture and conversion.