Epitaxial lateral overgrowth (ELO) of 1.8-μm InP films was performed on nanopatterned GaAs (001) substrates via metal–organic chemical vapor deposition. Parallel SiO2 trenches with a nano-scale width (∼ 170 nm) and various seed line orientations of [110], [410], [010] and [4–10] were first adopted to optimize the growth in our work. Scanning electron microscopy, atomic force microscopy and double-crystal x-ray diffraction were used to characterize the as-grown InP/GaAs heterostructures. The results reveal that the surface morphology and crystalline quality are strongly affected by the seed line orientations, and both of these parameters are optimized under the orientation of the [4–10] direction. A low average full width at half maximum of 285.1 arcsec and a root mean square surface roughness of 2.95 nm are obtained for the 1.8-μm InP film. To clearly observe the initial coalescence stage during the growth processes, thinner (500 nm) ELO InP films were also grown. We found that the seed line orientation has a significant effect on the lateral growth rate and affects the quality of the final InP/GaAs epilayer.