ABSTRACT Excess molar volume, excess isentropic compressibility, deviation in viscosity, and excess Gibbs free energy of activation of viscous flow for binary mixtures of Hexylene glycol (2-methyl-pentanediol-2,4 or MPD) with aliphatic ketones (4-hydroxy-4-methyl-pentan-2-one (J1), 4-methyl-pentan-2-one (J2), and pentan-2-one (J3)) components selected compositions were determined from the measured values of densities (ρ), viscosities (η), and speeds of sound (u) of pure components and their mixtures from 303.15 K to 313.15 K. The results were analysed in terms of intermolecular interactions or hydrogen bonding or hetero-association interactions in the binary mixtures. Finally, the Prigogine-Flory-Patterson (PFP) theory is applied to identify the most predominant molecular interaction. The results of the Jouyban-Acree model are discussed in terms of mean relative deviation (MRDs) and individual relative deviation (IRD) between calculated and experimental densities, speeds of sound, and viscosities as an accuracy criterion.