We report that a high local strain was obtained for multilayer MoS2 nanoscrolls decorated with noble nanoparticles (Ag and Au NPs) using a rolling process beyond breaking or slipping of MoS2. The local strain was estimated through the bending strain in the nanoscrolls and the extent of coverage of Ag and Au NPs decorated on MoS2, exhibiting magnified surface-enhanced Raman scattering. TEM images showed that the MoS2-Ag and MoS2-Au nanoscrolls have a tube-like morphology decorated with NPs on the inner and outer sides of the MoS2 nanoscrolls. In the Raman spectra, we confirmed the red shift and broadness of the FWHM for nanoscrolls in the eigenvectors of the [Formula: see text] and [Formula: see text] modes. From the Grüneisen parameter γ and the shear deformation potential β, we obtained peak shifts of ∼4.9 cm-1/% at [Formula: see text] and ∼1.1 cm-1/% strain at [Formula: see text] for free-standing MoS2. According to the obtained relationship of the Raman shift and the induced uniaxial tensile strain, the [Formula: see text] and [Formula: see text] peaks shifted upwards to around -12.8 cm-1 and -2.9 cm-1, respectively, and can be converted to an induced uniaxial tensile strain of about 2.6% for MoS2-Ag nanoscrolls.