Abstract Synthesis and spectroscopic characterization of a low molecular mass organogelator based on alkyl chain‐substituted tricyanofuran hydrazone (TCFH) dyes are described for detecting organophosphorus based nerve agent mimic. The reactivity of the prepared TCFH‐based organogel towards diethylchlorophosphonate (DCP) has been examined in organic phases. TCFH chromophore showed a successful gelation ability of different organic solvents. In addition, responsiveness of TCFH to nerve agent mimic with a gel‐sol reversible switching was monitored associated with colorimetric shifting from yellow to blue. The supramolecular self‐assembly of TCFH occurs via van der Waals interactions as well as cooperative π‐π stacking leading to gel formation in organic solvents. Moreover, the existence of nerve agents‐based gases results in a remarkable variation in the rheological behavior of the tricyanofuran hydrazone‐based gel. Scanning electron microscopy (SEM) images demonstrated that the xerogel generated from n ‐propanol ( n ‐PrOH) is able to create fibrous supramolecular architecture with the ability for naked‐eye detection of a nerve agent mimic. The development of TCFH‐based supramolecular organogel in organic solvents was disturbed by the nerve agent mimic presenting a novel detection technique for organophosphorus warfare agents.