Social interactions involve an interplay between lower-level social perceptual biases and higher-level cognition and affect. One particularly important building block of social interaction is attention to others’ eyes. Previous research has found links between individual differences in eye-looking and complex social capacities, including empathy. Such research, however, has predominately used nonnaturalistic stimuli and has not addressed the directional relation between these processes. In this study, a large sample of adults (N = 164) were eye-tracked while watching naturalistic videos of complex social interactions. Additionally, participants completed measures of empathy and spontaneous and explicit mentalizing. To disentangle relations between variables, participants were assigned to one of three conditions: first, a baseline condition with no instructions; second, an eye-looking condition, where participants were told to look at the eyes of the characters; and, third, an empathy condition, where participants were told to become involved with the characters’ thoughts and feelings. In the baseline condition, we found no relation between mentalizing and eye-looking, yet found that eye-looking and empathy were positively related. Inducing one behavior, however, did not affect the other. That is, participants in the eye-looking condition showed increased eye-looking but not increased empathy, and participants in the empathy condition scored more highly on empathy and mentalizing measures with no corresponding changes in eye-looking. These results suggest that the relations between visual attention and social cognition are complex and difficult to manipulate. Future research should examine the developmental links between these behaviors, as understanding their emergence has implications for social disabilities and interventions.