Hydrogels based on p(4-VP) of different dimensions were prepared and, after chemical modification, were used in the removal of one of the most potent toxic materials, cyanide. Macro and micron p(4-VP) hydrogel swelling behavior was evaluated in various aquatic environments. HCl, bromoethane, 1-bromobutane, 1-bromohexane, and 2-bromoethylamine were used as quaternizing agents to generate positive charges on both p(4-VP) macrogels and microgels. The modified p(4-VP) macrogels and microgels were used in cyanide ion removal for the first time from aqueous environments. The p(4-VP)-HCl at macro and micro sizes removed almost 49 and 61 mg cyanide ions per gram hydrogel in deionized water after modification, respectively. Moreover, the absorption capacity of the modified p(4-VP) hydrogel did not change significantly in tap, drinking, and creek waters. Parameters that affect the absorption process, such as cyanide concentration, contact time, hydrogel amount, and contaminated water source, were investigated. Additionally, magnetic field responsive macro and micro p(4-VP) hydrogel composites provided many advantages, such as easy handling after cyanide absorption, e.g., ready removal of cyanide-loaded p(4-VP) composites with an externally applied magnetic field. Langmuir and Freundlich adsorption isotherms were applied to the data obtained for cyanide uptake from aqueous environments.