In this report, a cost-effective, environmentally friendly all-polymer porous solid desiccant was synthesized and tested for atmospheric water generation. Hydrogel1 was produced through free-radical solution copolymerization and then modified by incorporating hygroscopic salt at two concentrations (X molarity and Y molarity) into the matrix, resulting in Hydrogel2 and Hydrogel3. The materials (0.1 g of sample) could adsorb 37.8 mg, 15.1 mg, and 36.9 mg of moisture at 25 °C and 90% relative humidity within 40 hours. Remarkably, nearly 100% of the adsorbed water was released at 50 °C within 8 hours, demonstrating an impressively low regeneration temperature. From the measurements, it can be concluded that the hygroscopic salt negatively impacted the structure and sorption behaviour of the desiccants. Moreover, energy consumption analysis revealed that Hydrogel1 required 3.5% less energy (24W) than conventional desiccants available on the market, such as silica gels, various zeolites, and hygroscopic salts, at a moisture flow rate of 1 kg/h. Furthermore, minimal or no performance decline was observed over the adsorption-desorption cycles, and it can be stated that a not fully emptied state presented better results. When immersed in water to assess their full potential and eliminate mass transfer limitations, 1 g of Hydrogel1, Hydrogel2, and Hydrogel3 could adsorb an outstanding 62 g, 35 g, and 47 g of water. These findings highlight the material’s potential for practical applications and emphasize critical design constraints for future optimization.