Differential and integral cross section measurements, for incident electron energies in the 20–50 eV range, are reported for excitation of several composite vibrational modes in α-tetrahydrofurfuryl alcohol (THFA). Optimisation and frequency calculations, using GAUSSIAN 09 at the B3LYP/aug-cc-pVDZ level, were also undertaken for the two most abundant conformers of THFA, with results being reported for their respective mode classifications and excitation energies. Those calculations assisted us in the experimental assignments of the composite features observed in our measured energy loss spectra. There are, to the best of our knowledge, no other experimental or theoretical data currently available in the literature against which we can compare the present results.