Viscosities (η) and densities (ρ) of five binary mixtures of ethanenitrile with benzene and several substituted benzenes viz methylbenzene, 1,4-dimethylbenzene, chlorobenzene and 1,2-dichlorobenzene have been experimentally determined at 308.15 K. Viscosity deviations (∆η) from the linear blending rule have been evaluated for all the mixtures studied. These are small with a maximum negative deviation of about 6% for binary mixture with benzene and maximum positive deviation of about 3% for mixture with 1,4-dimethylbenzene. ∆η Values are fitted into RedlichKister equation and standard deviations in ∆η values, σ (∆η) have been evaluated. The correlating performance of several viscosity models such as Grunberg -Nissan, Katti and Chaudhari, Hind-McLaughlin -Ubbelohde and Sedgwick has been evaluated. Grunberg-Nissan viscosity model is suitable for viscosities of several binary systems studied. The results are discussed in terms of molecular interactions between the components of binary mixtures.