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Background Sexuality is an integral part of most intimate relationships and is associated with both positive and negative relational and health outcomes. Whereas such associations are well established, the question of how and for whom sexual aspects of the relationship positively or negatively impact relationship quality remains largely unanswered. Although historically, the topics of sexuality and intimate relationships have had their own, mostly separate research traditions, currently, a burgeoning body of research is attempting to unite the two fields. The current research project aims to contribute to this evolution by filling critical gaps in our understanding of the associations among sexual and nonsexual relationship processes and couples' relationship satisfaction. Most previous research has focused on self-report and individual-based assessments and variables. The current project examines dyad-based processes on the level of the individual as well as the couple and investigates the contributions of sexual behavior and sexual communication to relational well-being through a dyadic lens and by using both self-report and observational methods. The following four specific aims were pursued in this doctoral thesis: (1) Examine the importance of sexual frequency and sexual communication in young, mixed-sex couples in the early stages of their relationship; (2) Examine the associations between different sexual behaviors and relationship satisfaction and test the impact of individual variables (i.e., attachment) on these associations; (3) Examine the characteristics of observed couple communication behaviors during sexual and nonsexual discussions and their associations with relationship satisfaction; (4) Explore neurophysiological dimensions of sexual communication by examining the association between oxytocin and observed communication behaviors during sexual and nonsexual couple discussions. Methods Using a multimethod approach that includes questionnaires, observations, and hormone assays, we recruited and collected data in 126 young, mixed-sex couples in the early stages of their relationship (N = 252). Two laboratory visits were scheduled, the first to explain the study and to obtain blood samples, and the second to have couples complete questionnaires and participate in videotaped couple discussions, 7 minutes each, on a sexual and nonsexual topic. Communication behaviors were coded using an adaptation of the Specific Affect Coding System (SPAFF) and the System for Coding Interactions and Family Functioning (SCIFF). Oxytocin plasma levels were determined using enzyme-linked immunosorbent assays (ELISA). Analyses were guided by the actor-partner interdependence model (APIM). Results Though self-reported sexual frequency and sexual communication were associated with sexual satisfaction, sexual communication but not sexual frequency predicted relationship satisfaction (Aim 1). However, attachment dimensions moderated the association between sexual behavior and relationship satisfaction: In more anxiously attached individuals, sexual frequency did predict relationship satisfaction. Unexpectedly, when distinguishing between sexual and intimate behavior, a higher frequency of intimate behavior was also associated with greater relationship satisfaction, but only in avoidantly attached individuals. These findings call for a more differentiated approach to the study of sexuality in couples and are in line with prior findings showing that the impact of intimate and sexual behaviors on relationship satisfaction varies depending on attachment dimensions (Aim 2). To explore the qualities of dyadic communication, observed couple communication behaviors during sexual and nonsexual discussions were coded, and results indicated that sexual discussions were characterized by fewer negative and more positive (i.e., affectionate and validating) communication behaviors as compared to nonsexual discussions. We found gender differences in the association between observed negative behaviors during sexual discussions and relationship satisfaction, with only men's behaviors linking to their own and their partner's relationship dissatisfaction. Affectionate and validating behaviors predicted higher relationship satisfaction in one's partner, independent of gender or discussion topic (Aim 3). Finally, we found evidence for neurophysiological involvement in the sexual communication patterns of couples. Peripheral levels of plasma oxytocin were significantly associated with specifically observed validating behaviors during the sexual and not the nonsexual couple discussion (Aim 4). Conclusion We aimed to contribute to our understanding of the relevance of dyadic sexual behavior and sexual communication to relational well-being in the early stages of romantic relationships. In addition to individual-based factors (e.g., attachment) influencing the importance of different sexual behaviors to relational outcomes, our results highlight unique qualities of self-reported and observed sexual communication, as an important contributor to relationship satisfaction, with specific affective qualities and neurophysiological underpinnings. Our findings provide additional insight in the role of sexuality in the early stages of romantic relationships and provide a basis for further research on the importance of sexual behavior and sexual communication.