Densities and viscosities of the binary systems of phenylmethanol with 2-butanone were measured for the entire composition range at T = (303.15, 308.15, 313.15, 318.15, and 323.15) K and at the atmospheric pressure. The excess molar volumes were derived from the experimental data and were fitted with the Redlich-Kister equation to obtain their coefficients and standard deviations. The Grunberg-Nissan equation was used to correlate the viscosity data. Furthermore, kinematic viscosities were compared with those predicted by the UNIFAC-VISCO model. The cause of relatively large deviations between the experimental and predicted kinematic viscosities was explored by comparing the combinatorial and residual terms of the UNIFAC-VISCO model.