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Humans routinely extract important information from images and videos, relying on their gaze. In contrast, computational systems still have difficulty annotating important visual information in a human-like manner, in part because human gaze is often not included in the modeling process. Human input is also particularly relevant for processing and interpreting affective visual information. To address this challenge, we captured human gaze, spoken language, and facial expressions simultaneously in an experiment with visual stimuli characterized by subjective and affective content. Observers described the content of complex emotional images and videos depicting positive and negative scenarios and also their feelings about the imagery being viewed. We explore patterns of these modalities, for example by comparing the affective nature of participant-elicited linguistic tokens with image valence. Additionally, we expand a framework for generating automatic alignments between the gaze and spoken language modalities for visual annotation of images. Multimodal alignment is challenging due to their varying temporal offset. We explore alignment robustness when images have affective content and whether image valence influences alignment results. We also study if word frequency-based filtering impacts results, with both the unfiltered and filtered scenarios performing better than baseline comparisons, and with filtering resulting in a substantial decrease in alignment error rate. We provide visualizations of the resulting annotations from multimodal alignment. This work has implications for areas such as image understanding, media accessibility, and multimodal data fusion.