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Augmenting reality via head-mounted displays (HMD-AR) is an emerging technology in education. The interactivity provided by HMD-AR devices is particularly promising for learning, but presents a challenge to human activity recognition, especially with children. Recent technological advances regarding speech and gesture recognition concerning Microsoft’s HoloLens 2 may address this prevailing issue. In a within-subjects study with 47 elementary school children (2nd to 6th grade), we examined the usability of the HoloLens 2 using a standardized tutorial on multimodal interaction in AR. The overall system usability was rated “good”. However, several behavioral metrics indicated that specific interaction modes differed in their efficiency. The results are of major importance for the development of learning applications in HMD-AR as they partially deviate from previous findings. In particular, the well-functioning recognition of children’s voice commands that we observed represents a novelty. Furthermore, we found different interaction preferences in HMD-AR among the children. We also found the use of HMD-AR to have a positive effect on children’s activity-related achievement emotions. Overall, our findings can serve as a basis for determining general requirements, possibilities, and limitations of the implementation of educational HMD-AR environments in elementary school classrooms.