Two types of optical metamaterials operating at near-IR and mid-IR frequencies, respectively, have been designed, fabricated by nanoimprint lithography (NIL), and characterized by laser spectroscopic ellipsometry. The structure for the near-IR range was a metal/dielectric/metal stack fishnet structure that demonstrated negative permittivity and permeability in the same frequency region and hence exhibited a negative refractive index at a wavelength near 1.7 um. In the mid-IR range, the metamaterial was an ordered array of four-fold symmetric L-shaped resonators (LSRs) that showed both a dipole plasmon resonance resulting in negative permittivity and a magnetic resonance with negative permeability near wavelengths of 3.7 um and 5.25 um, respectively. The optical properties of both metamaterials are in agreement with theoretical predictions. This work demonstrates the feasibility of designing various optical negative-index metamaterials and fabricating them using the nanoimprint lithography as a low-cost, high-throughput fabrication approach.