Herein, we have reported particle-assisted ion-imprinted cryogels, which were synthesized by embedding finely crushed functional particles into cryogel structure under semifrozen conditions. These cryogels showed high adsorption efficiency and affinity against Cd-II ions. CdII adsorption performances were evaluated by varying some effective factors. In order to analyze the data, we applied Langmuir and Freundlich adsorption isotherms while using three different kinetic models, pseudo-first-order, pseudo-second-order, and WeberMorris as well. Also, the dimensionless equilibrium parameter (R-L), initial adsorption rate, and half-adsorption time were calculated. The results revealed that ion-imprinted-polymer (IIP) cryogels have homogeneously distributed cavities, which were formed by a particle-assisted imprinting process, and the theoretical maximum adsorption capacity (Q(max), 35.97 mu g/g) was very close to the experimental value (Q(eq), 32.15 mu g/g). In addition, R-L values for both IIP and nonimprinted-polymer cryogels showed favorability of the adsorption process, while kinetic models indicated that there were no diffusion limitations during the adsorption process, which means that the rate-limiting step was chemosorption of heavy-metal ions on binding sites (imprinted cavities or functional groups) with a high initial adsorption rate and a low half-adsorption time. Desorption, reusability, and selectivity studies were also conducted to state the performance of the cryogels. In conclusion, this promising approach provides a novel methodology for selective Cd-II removal from water sources.