This chapter discusses elicitation of knowledge in work process design and its requirements on socio-technical support instruments. It provides the conceptual underpinnings of the articulation and alignment processes of work process elicitation. We detail relevant insights from different disciplines such as social psychology, cognitive sciences, knowledge management, and computer-supported collaborative work. The individual mental model of accomplishing work tasks, as well as role awareness, is crucial for capturing situated and thus contextual work behavior. For aligning individual mental models, intangible information exchange, and implicit work knowledge needs to be externalized and combined with existing encoded work representations. Such an endeavor lays the ground for co-creating digital work settings and meta-cognitive potential for further developments, in particular, organization learning steps. This chapter provides a corresponding theory-based synthesis. It reflects on methodologically grounded designs of work support and organizational development processes.