A cucurbit[6]uril (CB[6]) based supramolecular assembly CB[6]-[NDS]2- (1, NDS = 2,6-naphthalenedisulfonic acid anion) was used to detect dyes such as reactive blue 19 (RB19), rhodamine B (RB), methyl orange (MO), methyl red (MR), and methyl violet (MV), and isoquinoline antibiotics such as berberine (BER) and palmatine (PAL) with detection limits of 143, 128, 374, 193, 305, 27 and 34 ppb, respectively. Simultaneously, 1 also displayed high adsorption abilities towards these organic molecules. These results indicate that 1 is a favorable material for the simultaneous selective detection and removal of specific dyes and antibiotics from water, being potentially useful in monitoring water quality and treating wastewater. The possible mechanisms of the detection and adsorption are also proposed.