Ultraclean graphene is essential for studying its intrinsic transport properties or fabricating high-performance electronic devices. Unfortunately, the contamination on graphene is unavoidable after microelectromechanical system processing. Here, we report an in situ current-annealing method for achieving ultraclean suspended monolayer graphene. The charge mobility of cleaned graphene reached a surprising 3.8 × 105 cm2 V−1 s−1, one of the highest values ever reported. For the first time, the process of current annealing was recorded under a high-resolution electron scanning microscope. It was demonstrated that temperature was the only dominant factor of the current-annealing process. Meanwhile, the mobility of suspended graphene was found to be highly sensitive to structural defects. The mobility decreased by a factor of over 100 after ion irradiation on graphene. The results revealed the underlying mechanism of current annealing on graphene and provided an effective means of preparing ultraclean graphene membranes.