The Chimpanzee Facial Action Coding System (ChimpFACS) is an objective, standardized observational tool for measuring facial movement in chimpanzees based on the well-known human Facial Action Coding System (FACS; P. Ekman & W. V. Friesen, 1978). This tool enables direct structural comparisons of facial expressions between humans and chimpanzees in terms of their common underlying musculature. Here the authors provide data on the first application of the ChimpFACS to validate existing categories of chimpanzee facial expressions using discriminant functions analyses. The ChimpFACS validated most existing expression categories (6 of 9) and, where the predicted group memberships were poor, the authors discuss potential problems with ChimpFACS and/or existing categorizations. The authors also report the prototypical movement configurations associated with these 6 expression categories. For all expressions, unique combinations of muscle movements were identified, and these are illustrated as peak intensity prototypical expression configurations. Finally, the authors suggest a potential homology between these prototypical chimpanzee expressions and human expressions based on structural similarities. These results contribute to our understanding of the evolution of emotional communication by suggesting several structural homologies between the facial expressions of chimpanzees and humans and facilitating future research.