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Bulk Nb superconducting radio-frequency (SRF) cavities are widely used in accelerators, and their accelerating gradient and general performance are limited by the superheating field (Bsh). To push the theoretical limit of the Bsh, new multilayer structures are required. We fabricated FeSe-coated Nb films using pulsed laser deposition, performed structural characterizations, and measured the transport and magnetic properties for this superconductor-superconductor bilayer structure with smooth surface. Additionally, the measured Bc1 of FeSe-coated Nb film is greatly enhanced, while the Bsh of the FeSe layer is expected to be higher than that of bulk Nb, yet the superconducting transition temperature (Tc) is less than 5 K. This work presents the first fabrication of a new coating layer: FeSe deposited on Nb, showing the possibility of using iron-based materials for multilayer structures in SRF cavities.