Nuclear spin – lattice relaxation times T1 of protons have been measured as a function of concentration at room temperature for H2O/CD3COCD3 and CH3COCH3/D2O solutions. The results show that T1 reaches a minimum at ~ 0.8 mole fraction of water in both solutions. This is interpreted in terms of molecular association between water and acetone molecules by hydrogen bonding.Theoretical values for (1/T1)rot and (1/T1)trans are also calculated from rotational and translational correlation times using Stokes' model and the microviscosity model. Comparison with the experimental T1's shows that both models are inadequate to describe the system.Contributions to the overall (1/T1) from (1/T1)rot and (1/T1)trans are analyzed. It is found that the rotational motion dominated the relaxation process. The use of two different interaction parameters λ and ηe to describe molecular association is discussed.