The optical properties of materials are of great significance for their device applications. Different numbers of krypton ions are doped into high-quality Zn-polar ZnO films fabricated by molecular beam epitaxy (MBE) on sapphire substrates through ion implantation. Krypton is chemically inert. The structures, morphologies, and optical properties of films are measured. The x-ray diffraction (XRD) spectra confirm the wurtzite structures of Zn-polar ZnO films. Atomic force microscopy (AFM) results show that the films have pit surface structure and higher roughness after Kr ion implantation. A detailed investigation of the optical properties is performed by using the absorption spectrum, photoluminescence (PL), and spectroscopic ellipsometry (SE). The absorption spectrum is measured by UV-visible spectrophotometer and the bandgap energy is estimated by the Tauc method. The results show that the absorption increases and the bandgap decreases after Kr ion implantation. Moreover, the Kr ion implantation concentration also affects the properties of the film. The ellipsometry results show that the films’ refractive index decreases with the Kr ion implantation concentration increasing. These results can conduce to the design and optimization of Kr ion-implanted polar ZnO films for optoelectronic applications.