Epitaxial La2/3Ca1/3MnO3 thin films grown on LaAlO3 (001) substrates were irradiated with low-energy 120-keV H+2 ions over doses ranging from 1012 ions/cm2 to 1017 ions/cm2. The irradiation suppresses the intrinsic insulator—metal (I—M) transition temperature and increases the resistance by reducing the crystallographic symmetry of the films. No irradiation-induced columnar defects were observed in any of the samples. The specific film irradiated at a critical dose around 8 × 1015 ions/cm2 is in a threshold state of the electric insulator where the I—M transition is absent. In an external field of 4 T or higher, the I—M transition is restored and thus an enormous magnetoresistance is observed, while a negative temperature coefficient resumes as the temperature is reduced further. Magnetic relaxation behavior is confirmed in this and other heavily irradiated samples. The results are interpreted in terms of the displacement of oxygen atoms provoked by ion irradiation and the resulting magnetic glassy state, which can be driven into a phase coexistence of metallic ferromagnetic droplets and the insulating glass matrix in a magnetic field.