Development of cost-effective, highly reproducible non-conventional fabrication techniques for anisotropic metal nanostructures is essential to realizing potential applications of plasmonic devices, photonic devices, and surface enhanced Raman scattering (SERS) phenomenon based sensors. This report highlights the fabrication of nanotriangle arrays via nanoimprinting to overcome difficulties in creating large-area SERS active substrates with uniform, reproducible Raman signals. Electron beam lithography of anisotropic nanostructures, formation of arrays of nanotriangles in silicon and the transfer of triangular shapes to polymethylmethacrylate (PMMA) sheets via nanoimprinting have not been reported elsewhere. The reuse of silicon masters offers potential for production of low cost SERS substrates. The SERS activity and reproducibility of nanotriangles are illustrated and a consistent average enhancement factor of up to ~2.9 × 1011, which is the highest value reported for a patterned SERS substrate, is achieved.