The grain size for polycrystalline GaN, grown in low-temperature gallium-rich conditions, is shown to be correlated to the oxygen content of the films. Films with lower oxygen content were observed to have larger crystals with an increased tendency to a single-preferred crystal orientation. Elastic recoil detection analysis with heavy ions (i.e., 200 MeV [sup 197] Au ions) was used to determine the composition of the GaN films grown for the study, including the hydrogen, carbon, gallium, nitrogen, and oxygen content. Atomic force microscopy and x-ray diffraction were used to study the sample morphology. From these measurements, the available surface area of the films was found to be sufficient for a significant proportion of the oxygen present in the films to segregate at the grain boundaries. This interpretation is consistent with earlier theoretical studies of the formation and segregation of the V[sub Ga]-(O[sub N])[sub 3] defect complex at dislocation sites in gallium-rich GaN. For this work, however, the defect complex is believed to segregate at the grain boundary of the polycrystalline GaN.