The waste vitrification of abandoned open sky vermiculite deposits has been considered by combining with a natural phosphate mineral residue. Several batches haven been designed from the composition system: Li2O-MgO-Al2O3-P2O5-SiO2 including some Fe2O3 and Fluoride. The resulting glasses are transparent and smooth green coloured, giving rise after TTT treatments to several opal, opaque glass-ceramics with iridescent surface. Full characterization has been carried out by XRD and electron microscopy with EDS, as well as by XPS spectroscopies, concluding that the main crystalline phases formed were alpha-cordierite and beta-spodumene. The surface of these glass-ceramics from vermiculiteamblygonite is enriched in Fe2O3. Compared to the parent glasses, the final glass-ceramics exhibited and improvement in fracture toughness.