The aim of the present thesis is to contribute towards a fundamental understanding of the relationship between synthesis, structure and properties of nanostructured thin films. This is achieved by the implementation of advanced characterization techniques, which allow the evaluation of microstructure and mechanical properties at the sub-micron scale and with high spatial resolution. The activities in this field concentrated on “home” laboratory as well as large scale facility based methods. Applying a cantilever bending technique to nanostructured thin films widened the application field of micromechanical tests to small scale samples with inhomogeneous character. The developed technique allows a reliable determination of values on their orientation related elastic modulus, fracture stress and fracture toughness. Scanning X-ray nanodiffraction, using beamlines at the synchrotron sources P03 Petra III / DESY and ID13 at ESRF, provide a new insight into the microstructure of thin films. The suggested technique is a powerful tool for local characterization of phases, texture and crystallite size as well as residual stresses of thin films. Depth-gradients of relations between deposition conditions and resulting microstructure can now be established. The new approaches allow a better understanding of structure-property relationships in nanostructured thin films as they can be combined with established characterization techniques, i.e. nanoindentation. This allows for example to determine the local relationship between the apparent hardness of a thin film and its microstructure. The now available characterization techniques provide the basis to understand the complex relationship between growth parameters, local microstructure and local mechanical properties of nanostructured thin films. Thus, they allow to understand the macroscopic behavior of nanostructured thin films and to design materials with exceptional performance.