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Analyzing different modalities of expression can provide insights into the ways that humans interpret, label, and react to images. Such insights have the potential not only to advance our understanding of how humans coordinate these expressive modalities but also to enhance existing methodologies for common AI tasks such as image annotation and classification. We conducted an experiment that co-captured the facial expressions, eye movements, and spoken language data that observers produce while examining images of varying emotional content and responding to description-oriented vs. affect-oriented questions about those images. We analyzed the facial expressions produced by the observers in order to determine the connection between those expressions and an image's emotional content. We also explored the relationship between the valence of an image and the verbal responses to that image, and how that relationship relates to the nature of the prompt, using low-level lexical features and more complex affective features extracted from the observers' verbal responses. Finally, in order to integrate this multimodal data, we extended an existing bitext alignment framework to create meaningful pairings between narrated observations about images and the image regions indicated by eye movement data. The resulting annotations of image regions with words from observers' responses demonstrate the potential of bitext alignment for multimodal data integration and, from an application perspective, for annotation of open-domain images. In addition, we found that while responses to affect-oriented questions appear useful for image understanding, their holistic nature seems less helpful for image region annotation.