We investigated the surface plasmon resonance (SPR) of aluminum (Al) thin films with varying refractive index of the environment near the films in the far‒ultraviolet (FUV, ≤ 200 nm) and deep‒ultraviolet (DUV, ≤ 300 nm) regions. By using our original FUV‒DUV spectrometer which adopts an attenuated total reflectance (ATR) system, the measurable wavelength range was down to the 180 nm, and the environment near the Al surface could be controlled. In addition, this spectrometer was equipped with a variable incident angle apparatus, which enabled us to measure the FUV‒DUV reflectance spectra (170–450 nm) with various incident angles ranging from 45° to 85°. Based on the obtained spectra, the dispersion relation of Al‒SPR in the FUV and DUV regions was obtained. In the presence of various liquids (HFIP, water, alcohols etc.) on the Al film, the angle and wavelength of the SPR became larger and longer, respectively, compared with those in the air (i.e., with no materials on the film). These shifts correspond well with the results of simulations performed according to the Fresnel equations, and can be used in the application of SPR sensors. FUV‒DUV‒SPR sensors (in particular, FUV‒SPR sensors) with tunable incident light wavelength have three experimental advantages compared with conventional visible‒SPR sensors, as discussed based on the Fresnel equations, i.e., higher sensitivity, more narrowly limited surface measurement, and better material selectivity.