Grid environments were initially intended to deal with issues surrounding computing-intensive applications. Today, however, the use of Grids has evolved to tackle new horizons such as managing large amounts of data and running business applications that support consumers and casual users. In particular, this evolution towards a general-purpose, Grid service-based infrastructure allows educational institutions to enhance e-learning technologies and innovate in e-learning experiences through the provision and mutualisation of various services. Grid technologies will likely become the Information and Communication Technologies backbone of tomorrow's elearning programmes due to their ability to handle and process data from a multitude of resources (i.e., sensors, data warehouses, etc.) and offer new learning experiences which do not exist without the Grid capabilities. To face these new challenges, we propose a service-oriented Grid architecture capable to deliver services that can be used in collaborative learning processes and virtual learning environments. The architecture not only supports the provision of basic e-learning services but also provides infrastructure services (e.g., storage, computational resources, and security services), which can be combined to build on-demand and customized e-learning scenarios. The architecture is self-managed and exhibits autonomic behaviour to adapt itself to environment changes and exempt non-IT people from managing technical issues.