ABSTRACT The high energy consumption during regeneration of CO 2 ‐rich amine solutions remains a major challenge for amine‐based carbon capture. However, the addition of solid–acid catalyst accelerates the slow CO 2 desorption process while reducing the energy consumption for regeneration of the amine‐rich solution. Herein, we developed Co and Cu bimetallic–modified attapulgite (ATP) solid–acid catalysts via impregnation to enable energy‐efficient CO 2 desorption. The optimized Co 2 –Cu 1 /ATP catalyst exhibited exceptional performance in regenerating CO 2 ‐rich monoethanolamine (MEA) solution (5 M) at 90°C, achieving a 171% increase in CO 2 desorption rate, a 287% enhancement in CO 2 desorption amount, and a 75.6% reduction in regeneration heat duty compared to non‐catalytic processes. Comprehensive characterization (x‐ray diffraction [XRD], Fourier transform infrared [FT‐IR], NH 3 ‐TPD, N 2 adsorption–desorption, scanning electron microscopy [SEM]/EDS, x‐ray photoelectron spectroscopy [XPS]) revealed that the synergy between Co 3 O 4 and CuO nanoparticles on ATP generated abundant strong acid sites and optimized mesoporous structure, facilitating proton transfer and carbamate decomposition. FT‐IR analysis confirmed the catalytic accelerating effect of catalysts on the conversion of intermediates. The catalyst maintained 83% activity after eight regeneration cycles due to robust Co–O–Si/Cu–O–Si metal‐support interactions. This work provides a cost‐effective strategy for low‐energy carbon capture, advancing industrial deployment of carbon capture, utilization, and storage (CCUS) technology.