We reported the design and fabrication of a C-60 derivative with a uracil-like unit (U-C-60), to form a bi-molecular building block with a C-60 derivative with a 2,6-bis (acylamino) pyridine unit (DAP-C-60) by complementary trident hydrogen-bonding array. By pre-organizing these two fullerene derivatives in solution, bimolecular blocks were formed via robust and highly directional trident hydrogen-bonding recognition between DAP-C-60 and U-C-60. Then, the bimolecular blocks were deposited on highly ordered pyrolytic graphite (HOPG). The structure of the monolayer was characterized using a scanning tunneling microscope. Well-ordered monolayer composed of the two fullerene derivatives of DAP-C-60 and U-C-60 was observed and the structure of the monolayer was modeled. (c) 2005 Elsevier B.V All rights reserved.