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Plasmonic nanogap-enhanced Raman scattering has attracted considerable attention in the fields of Raman-based bioanalytical applications and materials science. Various strategies have been proposed to prepare nanostructures with an inter- or intra-nanogap for fundamental study models or applications. This report focuses on recent advances in synthetic methods to fabricate intra-nanogap structures with diverse dimensions, with detailed focus on the theory and bioanalytical applications. Synthetic strategies ranging from the use of a sil