We present low-resolution optical spectroscopy and BVRI photometry of 453 candidate nearby stars drawn from the NLTT proper motion catalogue. The stars were selected based on optical/near-infrared colours, derived by combining the NLTT photographic data with photometry from the 2MASS Second Incremental Data Release. Based on the derived photometric and spectroscopic parallaxes, we identify 111 stars as lying within 20 parsecs of the Sun, including 9 stars with formal distance estimates of less than 10 parsecs. A further 53 stars have distance estimates within 1-sigma of our 20-parsec 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 20 parsecs, of which 195 are additions to nearby-star catalogues. Most of the newly-identified nearby stars have spectral types between M4 and M8.