This chapter recapitulates our work based on focused ion beam-induced deposition of ultrathin amorphous carbon (FIBID-C) patterns as a route towards the easy integration of carbon nanomaterials. The use of postdeposition thermal processing causes structural changes, chemical modifi cation, and tuning of functional properties of the as-deposited FIBID-C. Particularly, in combination with metals our approach allows obtaining site-specifi c graphene-like features on insulators. We explore how to convert FIBID-C into functional materials, namely, graphene-like layers or diamond-like coatings, or combination with various metals.First, we provide a general description of FIBID technique to frame the profuse detailed case of carbon deposition of ultrathin carbon micropatterns. Then, the study of the transformation of FIBID-C by thermal processing reveals the unique characteristics of the as-deposited materials and particularities of the metal-induced crystallization. A detailed section on Raman spectroscopy is included as it represents a powerful tool to identify any carbon form, from amorphous to perfectly crystalline,