Ink-jet printing of monolayer-capped gold nanoparticles is introduced as a versatile and highly efficient means to pattern the alignment of nematic liquid crystals. Any homeotropic alignment patterns can be created quickly ranging in size from 30 m (850 dpi) to several square inches, with high accuracy that does not deteriorate with time. Depending on the alignment underlayer, intermediate configurations between homeotropic and homogeneous are also feasible. Nematic liquid crystals with both positive and negative dielectric anisotropy can be switched by applying a DC or AC electric field in the printed vertical domains with the substrate configuration determining the electro-optic response.