The treatment of contaminants in water has become one of the most critical environmental issues today, especially oil‐ and dye‐pollutants in water, for which there is still no efficient and economical solution. A multifunctional phase‐selective organogel (tert‐butyl (S)‐(5‐amino‐1,5‐dioxo‐1‐(tetradecylamino)pentan‐2‐yl)carbamate, TBTC) is developed to remove oils and dyes from water. Benefiting from the significant van der Waals interaction between the long alkyl chain of TBTC and the oil, TBTC can rapidly disperse into the oil phase. Then, TBTC aggregates into fibers and solidifies oil through a repairable, dynamic, and balanced hydrogen bonding network, which can solidify and recover the spilled oil at room temperature. TBTC can also efficiently remove more than a dozen typical dye contaminants through a host–guest recognition mode. The mechanism of host–guest recognition is studied by experiment combined with multiscale calculations. Partial 1H VT NMR, FTIR, and XRD experiments have shown that the main driving force for TBTC gelation and host–guest recognition originates from interaction hydrogen bonding, are TBTC specifically recognizes dye molecules through weak hydrogen bonding interactions and rapidly aggregates to form precipitates. TBTC‐based organogel provides a potential solution for oil spill recovery and removal of dyes from water.