Research object was the cultivation of values of ESD through the SPEEs in Secondary Education of Heraklion, Crete (Greece) prefecture. The values of ESD, and the followed methodology, for the cultivation of future environmentally literate citizens in the studied SPEEs constituted the Tool of Content Analysis, which applied to the projects’ archival material, to meet the aims of the research, to answer the research questions. There were sought references from the application forms and the final reports of the projects to some basic values that are enshrined in the Charter of Fundamental Rights (2000) of European Union and imported by UNECE strategy for ESD (2005) and Flogaiti (2006). These values were the ecological sustainability, social justice, autonomy, responsibility and tolerance, dignity, freedom, equality, solidarity, accountability and beauty sought to SPEEs as targets to be promoted and by what methodology. As the survey revealed, the teaching of values in schools with targeted projects and special methodology is in its infancy, at their very beginning stage. In the transformation of the EE Environmental Education to the Education for the Sustainable Development, school curriculum and educational projects need, immediately reconsideration and reconstruction to cultivate the future environmentally, scientifically, digitally literate active citizens.