The densities and viscosities of binary mixtures of isobutanol + cyclohexylamine have been measured over the entire range of composition at the various temperatures (293.15313.15 K) and at atmospheric pressure. From these measurements, the thermal expansion coefficients, isothermal coefficient of pressure excess molar enthalpy, excess molar volumes, and deviations in viscosities have been calculated too. The nonideality behavior of the mixture was evidenced in the excess molar volumes and deviations in viscosities. The results have been fitted to the RedlichKister polynomial equation. The GrunbergNissan equation was used to correlate the viscosity data. The most stable geometry of isobutanolisobutanol, cyclohexylamineisobutanol, and cyclohexylaminecyclohexylamine were studied using the density functional theory (DFT) in gases phase. In liquid phase, the molecular dynamics simulations have been performed and used to calculate the densities, mean square displacement (MSD), self-diffusion coefficients, and radial distribution functions of the mixtures with different mole fractions at 298.15 K and 1 atm. For these mixtures, using molecular dynamics simulation and quantum calculations, the structural and dynamical hydrogen bonding (H-bonding) interactions are considered too. These techniques are used to determine the hydrogen-bonded networks formed by the isobutanol and cyclohexylamine mixture.