(1) Background: Quality of care (QC) is not only about satisfying patients, but also about satisfying the various health system stakeholders (HSS). This makes it a complex and difficult objective to achieve. This study aims at proposing a methodological framework for identifying HSS, prioritizing them in QC, and analyzing their interrelationships. (2) Methods: The proposed framework is the mixed-method 5W2D approach, which uses a combination of three basic methods: the 5W questioning technique (What, Who, Why, Where, and When), the Delphi method, and the Decision making trial and evaluation laboratory (DEMATEL) technique. It consists of three interdependent phases. First of all, a preliminary list of HSS is established based on a systematic literature review, which is then projected and adapted to the national context using the 5W questioning technique. Secondly, the identified HSS are classified in order according to their influence and impact on QC by employing Delphi method. Thirdly, the interrelationships between HSS are determined and analyzed by applying DEMATEL technique. An application of 5W2D is conducted in the Moroccan context as its health system involves a wide range of stakeholders. (3) Results: Results defined 17 groups of HSS, whose prioritization led to three groups that are at the core of the health system: patients and their families, health personnel, and government. Roles and expectations of these groups regarding QC are divergent and contradictory, which require making trade-offs. The findings of this study intend to guide the development of inclusive strategies and policies that involve key stakeholders for QC assessment and improvement.