The parameters of molecular motion and physicochemical characteristics of disperse petroleum systems necessary to improve technologies of their processing are determined from the experimental relationships obtained using structural dynamic analysis by the pulse NMR technique. The revealed anomalies of the temperature relationships of the NMR and physicochemical parameters of molecular motion in the form of phase transitions in heavy oil and oil residues are caused by the dynamic ordering of aliphatic chains and aromatic hydrocarbons in the environment of the core of the complex structural unit of a disperse petroleum system. Changes in interproton distances during phase transitions arc calculated. Exchange between solvation-shell protons and dispersion-medium protons in crude oils and oil residues was revealed. A structural dynamic model for the complex structural units of petroleum was proposed, and the shortening of relaxation times in the phase transition region was theoretically explained. The model agrees well with the experimental data obtained.