We present low-resolution optical spectroscopy and BVRI photometry of 453 candidate nearby stars drawn from the NLTT (<I/98>) proper-motion catalog. The stars were selected based on optical/near-infrared colors, derived by combining the NLTT photographic data with photometry from the 2MASS Second Incremental Data Release (<II/241>). Based on the derived photometric and spectroscopic parallaxes, we identify 111 stars as lying within 20pc of the Sun, including nine stars with formal distance estimates of less than 10pc. A further 53 stars have distance estimates within 1{sigma} of our 20pc limit. Almost all of those stars are additions to the nearby-star census. In total, our NLTT-based survey has so far identified 496 stars likely to be within 20pc, of which 195 are additions to nearby-star catalogs. Most of the newly identified nearby stars have spectral types between M4 and M8.