Highly concentrated water-in-oil emulsions incorporating multiwalled carbon nanotubes (MWCNTs) are prepared. Homogeneous and selective dispersions of MWCNTs throughout the oil phase of the emulsions are investigated. The practical insolubility of carbon nanotubes (CNTs) in aqueous and organic media necessitates the disentanglement of CNT "agglomerates" through the utilization of functionalized CNTs. The design and synthesis of two tetra-alkylated pyrene derivatives, namely, 1,3,6,8-tetra(oct-1-yn-1-yl)pyrene (TOPy) and 1,3,6,8-tetra(dodec-1-yn-1-yl)pyrene (TDPy), for the noncovalent organic modification of MWCNTs are reported. The modifier molecules are designed in such a manner that they facilitate an improved dispersion of individualized MWCNTs in the continuous-oil phase of the highly concentrated emulsion (HCE). Transmission electron microscopic analyses suggest that the alkylated pyrene molecules are adsorbed on the MWCNT surface, and their adsorption eventually results in the debundling of MWCNT agglomerates. Fourier transform infrared, Raman, and fluorescence spectroscopic analyses confirm the Ï€-Ï€ interaction between the alkylated pyrene molecules and MWCNTs. The noncovalent modification significantly improves the effective debundling and selective dispersion of MWCNTs in HCEs.