The emerging technology of direct air capture (DAC) holds promise for the extraction of CO 2 from the air, offering a potential avenue to reverse climate change. However, DAC is still in its early stages of development, particularly on the sorbent material side, and the long-term stability of sorbents remains inadequately understood. This study investigates the impact of thermal degradation, hydrothermal treatment, long-term cyclic operation, and extended aging over 3 years on amine-supported sorbents and its effect on the adsorption capacity at DAC conditions. Sorbents were synthesized through various methods (impregnation, chemical grafting, and in situ polymerization) into two supports: large-pore AlMCM-41 (LPAlSi) and mesoporous silica foam (MSF). LPAlSi support demonstrates superior stability compared to MSF support under thermal and hydrothermal treatments. Impregnated sorbents with physically bonded amines exhibit the lowest stability, with a significant amine loss during all treatments, confirmed through porosity analysis, thermogravimetric analysis (TGA) decomposition, scanning electron microscopy (SEM), and Fourier-transform infrared spectroscopy (FTIR). Additionally, they experience a notable 6% decrease in CO 2 uptake after 50 cycles. In contrast, chemically bonded amines through grafting and in situ polymerization display better stability due to stronger bonding, maintaining CO 2 uptake despite harsh treatments. In situ-polymerized sorbents into LPAlSi exhibit remarkable stability under thermal and hydrothermal treatments, experiencing drops of 17 and 27% over 3 days, respectively. Furthermore, they demonstrate outstanding stability over 50 cycles under DAC conditions, with only a 0.3% drop in CO 2 uptake. Extended aging of class III sorbent for 3 years indicates good stability in CO 2 uptake, with only an 11% drop compared to impregnated ones, which showed a larger decrease over a shorter time. The presented results suggest that in situ-polymerized amines into LPAlSi are promising materials for DAC, offering good capacity and significant long-term stability. With opportunities for further sorbent optimization, there is substantial potential to deploy DAC at a scalable level and mitigate global warming effects.