Provided is a method for easily preparing a substrate comprising a monocrystalline film thereon or thereabove with almost no crystal defects without using a special substrate. More specifically, provided is a method for preparing a substrate comprising a monocrystalline film formed on or above a handle substrate, the method comprising: a step A of providing a donor substrate and the handle substrate; a step B of growing a monocrystalline layer on the donor substrate; a step C of implanting ions into the monocrystalline layer on the donor substrate so as to form an ion-implanted layer; a step D of bonding a surface of the monocrystalline layer of the ion-implanted donor substrate to a surface of the handle substrate; and a step E of peeling the bonded donor substrate at the ion-implanted layer existing in the monocrystalline layer so as to form the monocrystalline film on or above the handle substrate; wherein at least the steps A to E are repeated by using the handle substrate having the monocrystalline film formed thereon or thereabove as a donor substrate.