This dataset contains Giant Nuclei Impactor (GNI) NaCl-equivalent Sea-Salt Size Distributions collected during the VOCALS (VAMOS Ocean-Cloud-Atmosphere-Land Study) campaign. Polycarbonate microscope slides were exposed in the free air stream outside the NSF/NCAR C-130 using the manual GNI stick. Giant sea-salt aerosol particles are efficiently captured onto the slides. The slides were subsequently stored in desiccated test tubes and transported to NCAR/EOL/RAF. The slides were analyzed in the NCAR/EOL/RAF GNI slide chamber, using a dual-optical microscope.  Slides were inserted into a humidified chamber with a relative humidity of about 90%. The images were analyzed using an automated edge detection algorithm, and using spherical cap geometry to determine the solution drop volume. Subsequently, the equivalent dry NaCl equivalent radius was determined using the Kohler equation for concentrated solutions, specifically Pruppacher and Klett, 1978, eq. 6.26b, using a full chemical potential calculation. For a detailed description, see a manuscript in preparation by Jensen et al., available from the author.