We report a multi-objective campaign of targeted 21 cm H I line observations of sources selected from the Arecibo Legacy Fast Arecibo L-band Feed Array (ALFALFA) survey and galaxies identified by their morphological and photometric properties in the Sloan Digital Sky Survey. The aims of this program have been (1) to confirm the reality of some ALFALFA sources whose enigmatic nature suggest additional multiwavelength observations; (2) to probe the low signal-to-noise ratio (S/N) regime, below the ALFALFA reliability limit; and (3) to explore the feasibility of using optical morphology, color, and surface brightness to identify gas-rich objects in the region of the Pisces-Perseus Supercluster (PPS) whose H I fluxes are below the ALFALFA sensitivity limit at that distance. As expected, the reliability of ALFALFA detections depends strongly on the S/N of the H I line signal and its coincidence with a probable stellar counterpart identified by its optical properties, suggestive of ongoing star formation. The identification of low-mass, star-forming populations enables targeted H I line observations to detect galaxies with H I line fluxes below the ALFALFA sensitivity limits in fixed local volumes (D<100 Mpc). The method explored here serves as the basis for extending the sample of gas-bearing objects as part of the ongoing Arecibo Pisces-Perseus Supercluster Survey (APPSS).