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Canine-assisted interactions (CAIs) have been explored to offer therapeutic benefits to human participants in various contexts, from addressing cancer-related fatigue to treating post-traumatic stress disorder. Despite their widespread adoption, there are still unresolved questions regarding the outcomes for both humans and animals involved in these interactions. Previous attempts to address these questions have suffered from core methodological weaknesses, especially due to absence of tools for an efficient objective evaluation and lack of focus on the canine perspective. In this article, we present a first-of-its-kind system and study to collect simultaneous and continuous physiological data from both of the CAI interactants. Motivated by our extensive field reviews and stakeholder feedback, this comprehensive wearable system is composed of custom-designed and commercially available sensor devices. We performed a repeated-measures pilot study, to combine data collected via this system with a novel dyadic behavioral coding method and short- and long-term surveys. We evaluated these multimodal data streams independently, and we further correlated the psychological, physiological, and behavioral metrics to better elucidate the outcomes and dynamics of CAIs. Confirming previous field results, human electrodermal activity is the measure most strongly distinguished between the dyads’ non-interaction and interaction periods. Valence, arousal, and the positive affect of the human participant significantly increased during interaction with the canine participant. Also, we observed in our pilot study that (a) the canine heart rate was more dynamic than the human’s during interactions, (b) the surveys proved to be the best indicator of the subjects’ affective state, and (c) the behavior coding approaches best tracked the bond quality between the interacting dyads. Notably, we found that most of the interaction sessions were characterized by extended neutral periods with some positive and negative peaks, where the bonded pairs might display decreased behavioral synchrony. We also present three new representations of the internal and overall dynamics of CAIs for adoption by the broader field. Lastly, this paper discusses ongoing options for further dyadic analysis, interspecies emotion prediction, integration of contextually relevant environmental data, and standardization of human–animal interaction equipment and analytical approaches. Altogether, this work takes a significant step forward on a promising path to our better understanding of how CAIs improve well-being and how interspecies psychophysiological states can be appropriately measured.