Background: Since social cognition is impaired in individuals with autism spectrum disorder (ASD), this study aimed at establishing the efficacy of a newly developed imitation- and synchronization-based dance/movement intervention (SI-DMI) in fostering emotion inference and empathic feelings (emotional reaction to feelings of others) in adults with high-functioning ASD. Methods: Fifty-five adults with ASD (IQ ≥85) who were blinded to the aim of the study were assigned to receive either 10 weeks of a dance/movement intervention focusing on interpersonal movement imitation and synchronization (SI-DMI, n = 27) or a control movement intervention (CMI, n = 24) focusing on individual motor coordination (2 participants from each group declined before baseline testing). The primary outcome measure was the objective Multifaceted Empathy Test targeting emotion inference and empathic feelings. Secondary outcomes were scores on the self-rated Interpersonal Reactivity Index. The well-established automatic imitation task and synchronization finger-tapping task were used to quantify effects on imitation and synchronization functions, complemented by the more naturalistic Assessment of Spontaneous Interaction in Movement. Results: Intention-to-treat analyses revealed that from baseline to 3 months, patients treated with SI-DMI showed a significantly larger improvement in emotion inference (d = 0.58), but not empathic feelings, than those treated with CMI (d = -0.04). On the close generalization level, SI-DMI increased synchronization skills and imitation tendencies, as well as whole-body imitation/synchronization and movement reciprocity/dialogue, compared to CMI. Conclusions: SI-DMI can be successful in promoting emotion inference in adults with ASD and warrants further investigation.