Business-IT alignment is a crucial concept in the understanding of how profit-and-loss organizations use Information Technology (IT) to support their business requirements. This alignment concept becomes tangled when it is addressed in a socio-political context with non-financial goals and political agendas between independent organizations, i.e., in governmental settings. Collaborative problem-solving and coordination mechanisms are enabling government agencies to deal with such a complex alignment. In this chapter, the authors propose to consider four key domains for successful business-IT alignment in cross-governmental partnerships: partnering structure, IS architecture, process architecture, and coordination. Their choice of domains is based on three case studies carried out in cross-governmental partnerships, in Mexico, The Netherlands, and Canada, respectively. The business-IT alignment domains presented in this chapter can guide cross-governmental partnerships in their efforts to achieve alignment. Those domains are still open to further empirical confirmation or refutation. Although much more research is required on this important topic for governments, the authors hope that their study contributes to the pool of knowledge in this relevant research stream.