2H–13C HETCOR MAS NMR is performed on 2H/13C/15N-Pro enriched A. aurantia dragline silk. Proline dynamics are extracted from 2H NMR line shapes and T1 in a site-specific manner to elucidate the backbone and side chain molecular dynamics for the MaSp2 GPGXX β-turn regions for spider dragline silk in the dry and wet, supercontracted states.