Many health literacy interventions have a limited focus on functional/cognitive skills. In psychosocial models, the capacity to act however is seen as a major driver of behavioural change. This aspect is often lacking in health literacy concepts. In this study, we examine the impact of both aspects of health literacy (functional/cognitive and capacity to act) on specific healthcare outcomes (healthcare use, experiences with patient-centered care, shared-decision making, and self-management). In a sample of a national panel of people with a chronic disease (NPCD), questions about health literacy, patient activation, and outcomes were asked. The results indicated that 39.9% had limited HL levels and 36.9% had a low activation score. Combined, 22.7% of the sample scored low on both aspects, whereas 45.8% had adequate levels on both. Patients who score low on both use more healthcare and have less positive experiences with patient-centered care, shared decision making, and self-management. Patients who have adequate competency levels in both respects have the best outcomes. Both cognitive and non-cognitive aspects of health literacy are important, and they enhance each other. The capacity to act is especially important for the extent to which people feel able to self-manage.