Artificially structured materials, which are treated as macroscopically homogeneous media, exhibit effective optical properties that can be altered by engineering the materials' intrinsic geometries at a scale much smaller than the probing electromagnetic radiation at the wavelength of interest. Synthesizing structured optical materials to gain a variety of desired optical responses have flourished during the last decade thanks to the emergence of novel fabrication techniques like two-photon polymerization, for instance. Despite these advancements, there are still knowledge gaps regarding the optical properties of the polymers compatible with two-photon polymerization techniques. Representative examples demonstrating the potential of two-photon polymerization for the fabrication of all-dielectric optical metamaterials have not been extensively explored yet.This dissertation focuses on the development of all-dielectric metamaterials with structural features at sub-wavelength scales by using two-photon polymerization in order to engineer the material's dielectric properties at optical frequencies. In order to understand the optical responses of the all-dielectric metamaterials developed here, we accurately determined the optical properties of several two-photon polymerized polymers using spectroscopic ellipsometry over a spectral range from the ultraviolet to the near-infrared for the first time. Two different structured material classes composed of the investigated polymers were fabricated. These materials were designed to suppress Fresnel reflection loss or achieve very high reflection, respectively, at telecommunication wavelengths.The two-photo polymerization technique was further used to integrate engineered optical structures into the fabrication of opto-echanical components. We established a protocol for the rapid prototyping of functional opto-mechanical components. As an example, microlenses with anti-reflective structures conformally coated on concave lens interfaces and opto-mechanical components with critical features from the nm- to the mm-range have been fabricated in order to demonstrate our approach.