The Children and Families Act (2014) placed a statutory responsibility on local authorities in the UK to establish a virtual school headteacher with the role of championing the education of all children looked-after within that authority. The current research was designed to illuminate how virtual schools are currently supporting educational outcomes for children looked-after, not only through educational interventions, but also through supporting broader psychological factors that might impact on attainment such as attachment, relationships and mental health. Virtual school headteachers from 29 local authorities completed an online survey about the services they provided to three target groups—children looked-after, foster carers and schools—with a particular focus on the transition years from primary to secondary school, which have been identified as being a difficult time for children looked-after. Using inductive thematic analysis, four overarching themes to service provision were identified: enhanced learning opportunities, specific transition support, well-being and relationships, and raising awareness. Direct work, interprofessional working and the development of supportive environments, particularly guided by attachment theory, were identified as important areas of practice. Practice is discussed in relation to resilience and ecological systems theory and suggestions for future research are identified.