Within the context of a Europe-wide project UNITE, a number of European partners set out to design, implement and validate a pedagogical framework (PF) for e- and m-Learning in secondary schools. The process of formulating and testing the PF was an evolutionary one that reflected the experiences and skills of the various European partners and secondary schools involved in the project. The framework involved pedagogies which underpin the teaching of subject matter in a number of European secondary schools as well as the ways in which learning is delivered and assessed. The PF represents an essential part of the e-Learning system conceptualization and development and offers sound concepts for the development of learning scenarios in order to enhance the learning experience of students in secondary schools. A five-component framework which, by means of its constituents, drives and guides the creation of e-Learning scenarios was designed and tested. It is composed of the pedagogical framework context, pedagogical approaches, assessment techniques, teacher education and national specifics and current pedagogical practices implemented in national curricula. A series of learning scenarios were created to test the PF in classrooms. A detailed exemplar of a scenario in practice is offered. An evaluation of the scenarios based on [Reeves, T. C., 1994. Evaluating what really matters in computer-based education. In M. Wild, D. Kirkpatrick (Eds.), "Computer education: new perspectives" (pp. 219-246). Perth, Australia: MASTEC] pedagogical dimensions revealed that UNITE is based on constructivist and cognitive foundations. With increased experience of the system the teachers' implementation of the pedagogical framework developed into increased mastery in the school context. Teachers from the second validation phase became more confident in their application of the framework principles and evaluated more positively the outcomes. This helped them to become more aware of the opportunities offered by the framework in their secondary school teaching. In order to bring this about the supports for change were put into place at the levels of pedagogical design, administrative support and the provision of the required resources and appropriate continuing professional development. The project has sought to create this support structure to ensure maximal benefits of the system for teaching and learning. Such a pedagogical support PF has offered scope for both collaborative and autonomous learning which have brought about value-added teaching and learning effects in the Europe-wide network of schools. (Contains 3 tables and 6 figures.)