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The study of epitaxial graphene layers grown on SiC by two techniques, namely, the traditional Si sublimation method and the recent chemical vapor deposition (CVD) using temperature induced shift of the Raman 2D line, is presented. The measurements of thermal shift rate of 2D line on 4 H-SiC(0001) allowed us to determine notable differences in interaction of graphene with SiC substrate. The obtained results show that graphene layers grown by Si sublimation of 4 H-SiC(0001) are pinned strongly to the substrate. In contrast, the layers of graphene grown on 4 H-SiC(0001) substrates by CVD showed much weaker pinning. It was found that the film consisting of two or three graphene layers grown by CVD was already unpinned and thus showing Raman shift expected for freestanding graphene. The obtained differences in pinning of epitaxial graphene layers are explained in terms of basic growth mechanism differences between these two methods: graphene growth by Si sublimation is a “bottom-up” process and by CVD—a “top-down” process. The obtained results show that the CVD method of growth is an alternative technology for producing high quality graphene structures on SiC.