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On the purpose of in-situ observation of in-plane structures in organic ultrathin films, we employed the new system of total reflection X-ray diffraction method combined with Organic Molecular Beam Deposition (TRXD-OMBD). In-plane structure of fullerene (C60) thin films on Ag (111) surface was examined in vacuo by using TRXD-OMBD method. It was revealed that in-plane structures of as-deposited C60 thin films were anisotropic and epitaxially-grown along to the Ag [110] direction in the film plane. Also, the dependence of thickness was examined by the measurements of the depth profile of in-plane structures. Consequently, it was revealed that in-plane structures near the surface of C60 thin films and the interface of films / substrates were different.