The growth and characterization of GaxIn1−xP (x=0.51, 0.65, 0.69) are described in this paper. The organometallic vapor-phase epitaxial (OMVPE) growth was carried out in an atomospheric pressure reactor using trimethylgallium (TMGa), trimethylindium (TMIn), and phosphine (PH3). GaAs and commercially available hydride vapor-phase epitaxial GaAs0.70P0.30 and GaAs0.61P0.39 were used as the substrates. The influence of growth temperature and V/III ratio on the properties of the OMVPE epilayers was studied. This resulted in the determination of an optimum growth temperature of 625 °C and an optimum V/III ratio range of 40–50. The results of the mismatch due to the different lattice constants of the GaxIn1−xP epilayer and the substrate were investigated. It was found that high-quality GaxIn1−xP epilayers can be obtained only when the mismatch ‖Δa/a0‖ is less than 1×10−3. Under the conditions mentioned above, epilayers were reproducibly obtained with featureless surface morphologies, and photoluminescence (PL) with high intensities and narrow half-widths (41–43 meV at 300 K). The dislocation etch pit densities ρ of Ga0.65In0.35P and Ga0.69In0.31P epilayers were 7.4–8.6×104 cm−2, grown lattice matched to GaAs1−yPy ( y=0.30, 0.39) substrates with ρ=6.4–7.5×105 cm−2. The degradation of PL intensity after annealing at temperatures between 400 and 600 °C in H2 or N2 indicates an increase in the surface recombination velocity for GaInP epilayers. Etching 30 Å from the surface was found to restore the original PL intensity.