The misalignment between information technology (IT) and institutions continues to be a major problem, more particularly in higher education institutions. This state leads to a lack of technology value addition and poor institutional performance. Prior studies proposed models and frameworks with various organizational practices of IT-Business alignment. However, similar research, considering higher education institutions, is scarce. Therefore, this study explores and identifies the dimensions and practices of IT-institutional alignment from a higher education context. An exploratory embedded multiple-case study strategy is used on the two largest universities in Rwanda and Mozambique. Document survey and interviews are used for data collection. The literature and 14 interviews were analyzed using a thematic analysis approach to identify patterns related to the alignment practices. This study identified 45 IT-alignment practices reflected from both institutions, and they are classified into six metrics as presented in the framework. Of these alignment practices, 27 reflect exceptionally the higher education context of teaching, learning, and research. The identified alignment practices can serve as a frame of reference for creating and assessing the alignment between technology and university activities in the case study of institutions or similar contexts. A statistical test and validation of these alignment practices are recommended.