The growth of monolayer MoS2 crystals on chemomechanically polished (CMP) N-polar GaN using PTAS-assisted chemical vapor deposition is demonstrated. The formation of monolayer MoS2 was initially prevented by the as-grown GaN’s large surface roughness. CMP reduces the roughness to 250 pm, enabling monolayer MoS2 triangles with edge lengths of 30 μm, a Raman peak separation of <20 cm–1, and an optical bandgap of 1.81 eV, which is on par with those obtained on smooth Ga-polar GaN. It is thus demonstrated that high-quality MoS2 monolayers can be obtained on N-polar GaN for future high-speed optoelectronic and quantum sensing applications.