A theoretical study is presented on the mechanism of OH reactions with three unsaturated aldehydes, relevant to atmospheric chemistry. Using acrolein as test molecule, several methods were tested in conjunction with the 6-311 ++ G(d,p) basis set. Based on the results from this study, the MPWB1K and M05-2X functionals were selected for the further study of acrolein, methacrolein and crotonaldehyde. All possible reaction channels have been modeled. Calculated overall rate coefficients at M05-2X/6-311 ++ G(d,p) are in excellent agreement with experimental data, supporting the proposed mechanisms. The previously proposed global mechanisms were confirmed, and specific mechanisms were identified. The causes of the mechanism for crotonaldehyde being different from the one of acrolein and methacrolein were clarified. The agreement between experiment and calculations validates the use of the chosen DFT methods for kinetic calculations, especially for large systems and cases in which spin contamination is an important issue.