We introduce the Baryon Oscillation Spectroscopic Survey (BOSS) Emission-Line Lens Survey GALaxy-Lyα EmitteR sYstems (BELLS GALLERY) Survey, which is a Hubble Space Telescope program to image a sample of galaxy-scale strong gravitational lens candidate systems with high-redshift Lyα emitters (LAEs) as the background sources. The goal of the BELLS GALLERY Survey is to illuminate dark substructures in galaxy-scale halos by exploiting the small-scale clumpiness of rest-frame far-UV emission in lensed LAEs, and to thereby constrain the slope and normalization of the substructure-mass function. In this paper, we describe in detail the spectroscopic strong-lens selection technique, which is based on methods adopted in the previous Sloan Lens ACS (SLACS) Survey, BELLS, and SLACS for the Masses Survey. We present the BELLS GALLERY sample of the 21 highest-quality galaxy–LAE candidates selected from ≈ 1.4× {10}6 galaxy spectra in the BOSS of the Sloan Digital Sky Survey III. These systems consist of massive galaxies at redshifts of approximately 0.5 strongly lensing LAEs at redshifts from 2–3. The compact nature of LAEs makes them an ideal probe of dark substructures, with a substructure-mass sensitivity that is unprecedented in other optical strong-lens samples. The magnification effect from lensing will also reveal the structure of LAEs below 100 pc scales, providing a detailed look at the sites of the most concentrated unobscured star formation in the universe. The source code used for candidate selection is available for download as a part of this release.