A model-based approach is proposed to objectively measure and classify vocal fold vibrations by left-right asymmetries along the anterior-posterior direction, especially in the case of nonstationary phonation. For this purpose, vocal fold dynamics are recorded in real time with a digital high-speed camera during phonation of sustained vowels as well as pitch raises. The dynamics of a multimass model with time-dependent parameters are matched to vocal fold vibrations extracted at dorsal, medial, and ventral positions by an automatic optimization procedure. The block-based optimization accounts for nonstationary vibrations and compares the vocal fold and model dynamics by wavelet coefficients. The optimization is verified with synthetically generated data sets and is applied to 40 clinical high-speed recordings comprising normal and pathological voice subjects. The resulting model parameters allow an intuitive visual assessment of vocal fold instabilities within an asymmetry diagram and are applicable to an objective quantification of asymmetries.