This dissertation describes methodology that significantly improves the state of femtosecond laser writing of metals. The developments address two major shortcomings: poor material quality, and limited 3D patterning capabilities. In two dimensions, we grow monocrystalline silver prisms through femtosecond laser irradiation. We thus demonstrate the ability to create high quality material (with limited number of domains), unlike published reports of 2D structures composed of nanoparticle aggregates. This development has broader implications beyond metal writing, as it demonstrates a one-step fabrication process to localize bottom-up growth of high quality monocrystalline material on a substrate. In three dimensions, we direct laser write fully disconnected 3D silver structures in a polymer matrix. Since the silver structures are embedded in a stable matrix, they are not required to be self-supported, enabling the one-step fabrication of 3D patterns of 3D metal structures that need-not be connected. We demonstrate sub-100-nm silver structures. This latter development addresses a broader limitation in fabrication technologies, where 3D patterning of metal structures is difficult. We demonstrate several 3D silver patterns that cannot be obtained through any other fabrication technique known to us. We expect these advances to contribute to the development of new devices in optics, plasmonics, and metamaterials. With further improvements in the fabrication methods, the list of potential applications broadens to include electronics (e.g. 3D microelectronic circuits), chemistry (e.g. catalysis), and biology (e.g. plasmonic biosensing). / Engineering and Applied Sciences