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Abstract Carbon materials derived from fullerene are reported recently with unique structures and properties. However, only micrometer size samples can be obtained that limits the studying and exploration for membrane applications. Here, the preparation of a centimeter‐size nanoporous amorphous carbon monolayer is reported by rapid pyrolyzing a Langmuir–Blodgett film of fullerene. The sample is fully characterized and the results indicate that the amorphous carbon monolayer derived from fullerene is metastable and insulating. The ionic transmembrane transport study demonstrates that the membrane is porous and cation selective with a selectivity of 26%. This work provides new insights into the controlled synthesis of large‐size metastable amorphous carbon monolayer.