A platform of polymeric cryogels based on methacrylic acid (C-mA) meglumine (C-megl), lysine (C-lys), and 2-hydroxy ethyl methacrylate (C-ph), as well as a combination thereof having both negatively and positively charged moieties, have been synthesized and used to efficiently remove emerging contaminants from water. Their peculiar properties in sequestering antibiotics (Levofloxacin, Ampicillin, Doxycycline), anti-inflammatory (Piroxicam), antifungal (Fluconazole), anti-parasite (Moxidectin), pesticides (2,4D) and dyes (Thymol blue, Methylene Violet) were tested taking into account their ionic nature in solution. The adsorption experiments performed in batches at different pH and pollutant concentrations have demonstrated the outstanding ability of these macroporous soft systems in complexing molecules by the instauration of various binding forces, also in the presence of inorganic species such as arsenic (as arseniate). In addition, it was demonstrated as the novel dual-material, ad-hoc synthesized by using opposite charge cryogels, can simultaneously remove antagonist dyes in a single and fast cycle. Besides, a quasi-total release of the target molecules was achieved by changing pH, allowing the regeneration of the macroporous sponges for multiple re-uses without losing their performance. The latter peculiar feature may be adopted for drug delivery applications since the release can be modulated and programmed by a specific pH stimulus.