LAUSR

Efficient capture and ultrasensitive detection of radioiodine from nuclear industrial waste and contaminated water are crucial for environmental safety, yet achieving both simultaneously with a single material remains challenging. Here, a tetrathiafulvalene (TTF)decorated organic cage (TTFcage) is reported that serves as a high-performance adsorbent for trace iodine (I2) in both industrial off-gas and polluted water, and as a molecular cagebased organic field-effect transistor (cOFET) for ultrasensitive I2 detection. TTFcage shows strong I2 affinity through cooperative charge-transfer interactions of N and S sites, resulting in an ultrahigh I2 vapor uptake of 1.28 g g-1 under >150 °C and <150 ppmv of I2 conditions, 7.1 times higher than industrial silver adsorbents. It also decontaminates iodine in flowing water below the secure criteria of World Health Organization (WHO, <0.1 ppm) with a high adsorption capacity of 5.16 g g-1. The electroactive TTF units impart tunable conductivity upon I2 binding, enabling an unreported cOFET sensor with a limit of detection (LoD) of I2 as low as 0.58 ppt (≈10-12 M), exceeding conventional spectroscopic methods by 6 orders of magnitude. Moreover, I2 adsorption and detection can be integrated into a miniaturized chip, providing a portable platform for on-site pollution treatment and synchronized environmental monitoring of radioiodine.