Infrared (IR) spectroscopy is a powerful technique for observing organic molecules, as it combines sensitive vibrational excitations with a non-destructive probe. However, gaseous volatile compounds in the air are challenging to detect, as they are not easy to immobilize in a sensing device and give enough signal by themselves. In this study, we fabricated a thin nanocrystalline metal-organic framework (nMOF) film on a surface plasmon resonance (SPR) substrate to enhance the IR vibration signal of the gaseous volatile compounds captured within the nMOF pores. Specifically, we synthesized nanocrystalline HKUST-1 (nHKUST-1) particles of ca. 80 nm diameter and used a colloidal dispersion of these particles to fabricate nHKUST-1 films by a spin-coating process. After finding that benzene was readily adsorbed onto nHKUST-1, an nHKUST-1 film deposited on a plasmonic Au substrate was successfully applied to the IR detection of gaseous benzene in air using surface-enhanced IR spectroscopy.