Proton dynamics in pristine and organically-modified layered double hydroxide has been studied by H-1 T-1 rho. Inverse Laplace transform with spectral resolution results in a correlation of T-1 rho and chemical shift. In LDH two contributions are resolved. They are assigned to the metal hydroxides, forming the LDH sheets (4-8 ms), and mobile interlayer water (2 ms). Apparent T-1 rho values of OH-protons in surfactant-modified LDH are different in dodecylbenzenesulfonate-(SDBS) and sodium octasulfonate-(C8) modified LDH. This difference is explained by the presence of water in LDH-SDBS. The effects of spin diffusion have been studied by performing 2D H-1 RFDR in the LDH-SDBS. (C) 2011 Elsevier B.V. All rights reserved.