Organic polymers are widely explored due to their high stability, scalability, and more facile modification properties. We developed cost-effective dithiocarbamate-based organic polymers synthesized using diamides, carbon disulfide, and diamines to apply for environmental remediation. The sequestration of radioiodine is a serious concern to tackle when dealing with nuclear power for energy requirements. However, many of the current sorbents have the problem of slower adsorption for removing iodine. In this report, we discuss the utilization of an electron-rich dithiocarbamate-based organic polymer for the removal of iodine in a very short time and with high uptake. Our material showed 2.8 g/g uptake of vapor iodine in 1 h, 915.19 mg/g uptake of iodine from cyclohexane within 5 s, 93% removal of saturated iodine from water in 1 min, and 1250 mg/g uptake of triiodide ions from water within 30 s. To the best of our knowledge, the iodine capture was faster than previously observed for any existing material. The material was fully recyclable when applied for up to four cycles. Hence, this dithiocarbamate-based polymer can be a promising system for the fast removal of various forms of iodine and, thus, enhance environmental security. © 2023 by the authors.