Carbon neutrality is one of the central topics of not only the scientific community but also the majority of human society. The development of highly efficient carbon dioxide (CO₂) capture and utilization (CCU) techniques is expected to stimulate routes and concepts to go beyond fossil fuels and provide more economic benefits for a carbon-neutral economy. While various single-carbon (C₁) and multi-carbon (C₂₊) products have been selectively produced to date, the scope of CCU can be further expanded to more valuable chemicals beyond simple carbon species by integration of nitrogenous reactants into CO₂ reduction. In this Review, research progress toward sustainable production of high-value-added chemicals (urea, methylamine, ethylamine, formamide, acetamide, and glycine) from catalytic coupling of CO₂ and nitrogenous small molecules (NH₃, N₂, NO₃^–, and NO₂^–) is highlighted. C–N bond formation is a key mechanistic step in N-integrated CO₂ reduction, so we focus on the possible pathways of C–N coupling starting from the CO₂ reduction and nitrogenous small molecules reduction processes as well as the catalytic attributes that enable the C–N coupling. We also propose research directions and prospects in the field, aiming to inspire future investigations and achieve comprehensive improvement of the performance and product scope of C–N coupling systems.