Inspired by an increasing demand for stimuli-controlled assembly of nanostructures, mechano-responsive nanocomposites are designed with tremendous scope in material applications. Providing switchable properties by means of mechanical stimulation, elastomer-incorporated gold nanorods (AuNR) are presented herein. Stepless and reversible control over the orientational AuNR alignment and therefore over macroscopic anisotropy - is exerted by uniaxial film elongation. In context of optical applications, substantial impact on the plasmonic properties within adjustable spectral ranges is demonstrated. Mechano-responsive nanocomposites with high thermal colloidal stability are prepared via a facile hetero-phase ligand exchange procedure where complete coverage of the AuNR surface with hydrophobic ligands is achieved. (C) 2015 Elsevier Ltd. All rights reserved.