A novel class of optical metamaterials is presented consisting of high densities of aligned gallium phosphide (GaP) nanowires fabricated using metal-organic vapor phase-epitaxy. Starting from a gold island film as a catalyst for nanowire growth, a sequential combination of vapor-liquid-solid and lateral growth modes is employed to obtain a continuous tunability of the nanowire volume fraction from 7% to over 35%., By choosing different crystallographic orientations of the GaP substrate, metamaterials are designed with different nanowire orientations. The anisotropy of the nanowire building blocks results in strong optical birefringence. Polarization interferometry demonstrates I a very large polarization extinction contrast of 4 x 103 combined with a sharp angular resonance which holds promise for optical sensing. Nanowire metamaterials may find applications in photonics, optoelectronics, non-linear and quantum optics, microfluidics, bio-, and gas sensing.