A diverse range of alkali/amine infused hydrogels (AIHs) were generated by incorporating the liquids into a hydrogel particle for carbon capture application. As a consequence, the CO2 uptake was significantly enhanced owing to the increased contact area. This AIHs technique was highly tunable as it could be applicable to varying species of alkali chemicals and it was found that their molecular structure and architectures could impact the CO2 uptake. Compared to stirred bulk alkali/amine solutions, the CO2 absorption capacity of AIHs was increased by 400% within 30 min with a low hydrogel loading (10 w/w%). In addition, the recyclability of various AIHs was assessed and was found to be extremely encouraging. The effect of salinity on the performance of AIHs was also investigated and high salinity was found to have a minimal effect on CO2 absorption. Most importantly, the preparation of AIHs is fast and straightforward with few wastes and byproducts formed in the preparation process. In all, extensive investigations were presented and the AIHs were found to be a highly tunable and effective approach to enhance CO2 capture with liquid alkali/amines.