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Vacuum filtration enables the fabrication of large-area graphene-based membranes (GBMs), possessing a smoother surface than that by spray, spin coating or drop casting. However, due to the strong interaction with substrates, the separation of thin GBMs from the filter is problematic. Conventional stamping separation/transfer of graphene oxide (GO) thin films requires another substrate and pressing for >10 h, which may damage the delicate structure of the transfer substrates. Other methods require GO to be reduced on filters before separation, thus limiting the reduction methods. Inspired by a coagulation bath that enables rapid formation of ultrastrong GO fibers, we present an ultrafast (<1 min) and solution-assisted strategy to fabricate smooth and freestanding GO films. The diverse interfacial energy of hydrogen bonds also demonstrates another reason for the successful separation. The film thickness ranges from 45 nm to several micrometers. When used as a composite of counter electrodes in dye sensitized solar cells, it showed higher (8.58%) power conversion efficiency than its spin-(7.71%) and spray-coated (8.07%) counterparts. It also showed promising performance in capacitive humidity sensors. The capacitance varied by three orders of magnitude in the range of the relative humidity of 15%-95%. Therefore the strategy realizes an ultrafast and high-quality film production which is suitable for various applications.