The two crystallographically distinct sites in Rb2CrO4 are characterized in terms of their Rb-87 quadrupole coupling and chemical shielding anisotropy (CSA) interactions employing Rb-87 single-crystal NMR. Accurate values for the quadrupole coupling and CSA parameters are reported for both rubidium sites along with the direction cosines describing the orientation of the tensors for the NMR interactions with respect to the Rb2CrO4 crystal frame. The parameters for site 1 represent the first accurate investigation of this site, while the parameters for site 2 compare excellently with those previously reported. Some remarkable similarities are observed between the present parameters for Rb2CrO4 and the Cs-133 parameters determined from recent magic-angle spinning and single-crystal Cs-133 NMR studies for the isomorphous Cs2CrO4.