High-quality GaN layers were grown on sapphire (0001) substrates using laser molecular beam epitaxy (LMBE) by laser ablating a solid GaN target at different laser repetition rates (10–40 Hz) under a constant supply of r.f. nitrogen plasma. The effect of laser repetition rate on the structural and optical properties of GaN layers was systematically studied using high-resolution X-ray diffraction (HRXRD), field emission scanning electron microscopy, atomic force microscopy, Raman spectroscopy and photoluminescence (PL) spectroscopy. High-resolution X-ray rocking curve measurements revealed highly c-axis oriented GaN layers on sapphire grown at 30 Hz with a calculated screw dislocation density of ~1.42 × 107 cm−2, whereas the GaN layers grown at 10 or 40 Hz consisted the screw dislocation density in the range of 108–109 cm−2. Surface morphological analysis revealed a change in grain size as well as surface roughness as a function of laser repetition rate and is explained on the basis of growth kinetics. Vibrational Raman spectroscopy revealed that the GaN layer grown at 10 Hz shows an in-plane compressive stress of ~1 GPa, while the film grown at 30 Hz exhibits a minimum stress of ~0.3 GPa. The PL measurements show a highly luminescent band-to-band emission of GaN at 3.44 eV for the 10 Hz grown highly strained GaN layer and at 3.41 eV for the less strained film grown at 30 Hz along with a broad defect band emission centered around 2.28 eV. It is found that the GaN layers grown at 30 Hz have excellent structural and optical properties. We expect that the less strained thin and highly oriented GaN film grown by LMBE can further be utilized for developing prodigious low-temperature-grown nitride-based multilayer structures and devices.