By UV-vis absorption and fluorescence spectroscopy it has been established that 25,27-dihydroxy-26,28dimethoxycalix[4]arene (1) forms reverse micelles in CCl4 and n-hexane media. The new feature of this compound as a surfactant is that even before micelle formation it can incorporate water molecules and the critical micellization concentration (cmc) in nonaqueous media increases with increase in omega (=water: 1 mole ratio). The inclusion complex of 1 with [70]fullerene has a CT absorption band that, in conjunction with those of some quinone complexes of 1, leads to the determination of the vertical ionization potential of 1. H-1 NMR spectrometric determination of the formation constant (K) of the inclusion complex of [60]fullerene with 1 in CCl4 has revealed that K increases on addition of microquantities of water. This has been rationalized by assuming that the -OH groups of the calix[4]arene molecules attach themselves to the water micropool of the reverse micelles by forming H-bonds and the individual calix[4]arene molecule obtains a conical conformation with a wider rim diameter than that in the absence of water and that this preorganization facilitates inclusion. By utilizing the spectral variation of the [60]fullerene.1 complex in CCl4 as the continuous medium with change in omega, a critical omega (=8) has been found below which the water in the micropool is "bound" and above which "free" water begins to accumulate in the water micropool.