Theoretical conceptualizations of mentalizing postulate a close relationship between the ability to mentalize and the regulation of emotional states. The former is viewed as a key process to modulate the latter, with the origins of the link between the two established in early attachment relationships. However, there is a lack of research testing this association empirically. In the present cross-sectional study, the hypothesis of a positive relationship between the two constructs was tested based on data collected on more than 500 nonclinical adult participants. Various self-assessments and an experimentally derived instrument of mentalizing were employed to this end. Correlational analyses confirmed the expected associations between emotion regulation and mentalizing. In addition, regression models showed that adaptive as well as maladaptive emotion regulation, independent of age, gender, and native language, could be predicted only by self-focused mentalizing.