Conventional interfacial polymerization (IP) encounters significant challenges in achieving the desired nanofiltration (NF) membrane structure, owing to uncontrolled diffusion and ultrafast polymerization. Our study introduced carbonates into the low-temperature interfacial polymerization (LTIP) process to precisely regulate the diffusion of amine monomers and polymerization kinetics. Carbonates in the aqueous phase restrict the diffusion of amine monomers while promoting the generation of nanobubbles. Further utilization of the low-temperature oil phase not only retards polymerization but also facilitates the formation of foam nanostructures in the polyamide layer. Density functional theory calculations and molecular dynamics simulations revealed the mechanisms underlying the regulation of amine monomer diffusion and gas-bubble release by carbonates and LTIP. The fabricated membrane has a smoother, ultrathin separation layer while maintaining a high permeability of 35.0 L·m−2·h−1·bar−1 (nearly doubled compared with the pristine membrane) and high Na2SO4 rejection of 99.5 %. This study confirms the practicality of the carbonate-modulated LTIP strategy.