A biocompatible, reliable, fast, and nanomolar-level dual-functional sensor for a neurotransmitter (e.g., adrenaline) and an anti-cancer drug (e.g., 6-mercaptopurine (6-MP)) is still far away from the hand of modern-day researchers. To address this issue, we synthesized an aqua-stable, bio-friendly, thioureafunctionalized Zr(IV) metal−organic framework (MOF) for selective, rapid sensing of adrenaline and 6-MP with ultra-low limit of detection (LOD for adrenaline = 1.9 nM and LOD for 6-MP = 28 pM). This is the first MOF-based fluorescent sensor of both the targeted analytes. The sensor not only can detect adrenaline in HEPES buffer medium but also in different bio-fluids (e.g., human urine and blood serum) and pH media. It also exhibited 6-MP sensing ability in aqueous medium and in various wastewater specimens and pH solutions. For the quick and on-site detection of this neuro-messenger (adrenaline) and the drug (6-MP), cost-effective sensor-coated cotton fabric composites were fabricated. The MOF@cotton fabric composite is capable of detecting both the analytes up to the nanomolar level by the naked eye under UV light. The sensor can be recycled up to five times without significantly losing its efficiency. The Forster resonance energy transfer in the presence of adrenaline and inner-filter effect in the presence of 6-MP are the most likely reasons behind the quenching of the MOF's fluorescence intensity, which were proved with the help of appropriate instrumental techniques.