To date, studies focusing on the connection between psychological functioning and autonomic nervous system (ANS) activity usually adopted the one-dimensional model of autonomic balance, according to which activation of one branch of the ANS is accompanied by an inhibition of the other. However, the sympathetic and parasympathetic branches also activate independently; thus, co-activation and co-inhibition may occur. The autonomic balance and regulatory capacity model accounts for such a diversity of autonomic activities. In the present study, we adopted a refinement of this model to assess how markers of the autonomic space relate to several critical psychological constructs: emotional contagion (EC), general anxiety, and positive and negative affect (PA and NA). We analyzed data from 408 healthy students, who underwent a 5-minute baseline period as part of their participation in several experiments and then completed self-reported questionnaires. During the baseline, electrocardiogram (ECG), electrodermal activity (EDA), and respiratory activity were recorded. Respiratory sinus arrhythmia (RSA), as well as cross-system autonomic balance (CSAB) and regulation (CSAR), were calculated. A comparison between psychological and physiological indices revealed distinct patterns of psychological associations for each physiological index: CSAB was positively correlated with EC and negatively correlated with PA and NA. Negative associations were noted between CSAR and EC. EDA was positively correlated with PA and NA and negatively linked to EC. We thus provide support for using the two-dimensional autonomic space framework in psychophysiological research. The advantages of the autonomic balance and regulatory capacity model are discussed.