We studied the relationship of respiratory sinus arrhythmia (RSA) to the co-activation of autonomic and facial expressive responses in 37 adult men during Rorschach testing. Interbeat interval (IBI), electrodermal activity, and facial electromyography were recorded continuously during the experiment. Prevailing mood and variability in the experience of valence and arousal were also measured. Bivariate intraindividual time series analysis was used to quantify spontaneously coupled phasic physiological responses. The results suggested that (a) spontaneous autonomic and expressive responses tend to parallel in time; (b) baseline, task-level, and task-induced change of RSA were positively related to coupled autonomic–expressive responses, a change in mood toward a more energetic state, and a tendency to have more variability in the emotional experience during the task; and (c) especially cardiac–expressive response coupling was related to mood change. It is concluded that the vagal system is related to the control of facial muscle activity and may mediate both tonic and phasic emotion-related changes in IBI. The role of phasic intraindividual response patterns in emotional and social behavior is highlighted.