Urea is widely used in fertilizer production for agricultural purposes which risks runoff into soil and water sources. An excess of urea can result in algal or toxic blooms which can poison wildlife or even humans by accumulation in food sources. The removal of urea from water is challenging due to the small size (0.254 nm) and uncharged surface of urea. Intensive research has been conducted on a variety of methods to remove environmental concentrations of urea using adsorbents, but most of them lack effective removal, require long (>2 h) process time, and lack re-generability. Metal-organic frameworks (MOFs) are the new generation of adsorbents with excellent structural and functional group tunability. In this study, we synthesized MIL-100 (Fe), an iron-based MOF, as an efficient adsorbent for the removal of uncharged urea from water. The urea adsorption capacity of MIL-100 (Fe) was tested under varying experimental conditions such as pH (2–10), temperature (25–65 °C), MOF concentration (25–400 ppm), and urea concentration (25–1000 ppm). The results showed the superfast adsorption (more than 85% removal within 2 min) of neutrally charged urea molecules on MIL-100 (Fe). The MOF was able to reach a maximum adsorption efficiency of around 85% with a maximum uptake capacity of 3321 mg/g. The MIL-100 (Fe) showed acceptable re-generability by retaining up to 90% removal efficiency after four regeneration cycles. The urea adsorption followed pseudo 2nd-order adsorption kinetics and dipole-dipole interactions and π-NH bonding were the primary adsorption mechanism.