Young stars in the solar neighborhood serve as nearby probes of stellar evolution and represent promising targets to directly image self-luminous giant planets. We have carried out an all-sky search for late-type (≈K7-M5) stars within 100 pc selected primarily on the basis of activity indicators from GALEX and ROSAT . Approximately two thousand active and potentially young stars are identified, over 600 of which we have followed up with low-resolution optical spectroscopy and over 1000 with diffraction-limited imaging using Robo-AO at the Palomar 1.5-m telescope. Strong lithium is present in 58 stars, implying ages spanning ≈10-200 Myr. Most of these lithium-rich stars are new or previously known members of young moving groups including TWA, β Pic, Tuc-Hor, Carina, Columba, Argus, AB Dor, Upper Centaurus Lupus, and Lower Centaurus Crux; the rest appear to be young low-mass stars without connections to established kinematic groups. Over 200 close binaries are identified down to 0. 2 -the vast majority of which are new -and will be valuable for dynamical mass measurements of young stars with continued orbit monitoring in the future.