<p>Recoil fast neutron spectroscopy with organic scintillators is hampered by the difficulty of its spectrum unfolding, which is caused by a flat response of the detectors to monoenergetic neutrons. Capture-gated (CG) fast neutron spectroscopy using composite scintillators is a promising method for addressing this problem as the CG events produce a characteristic peak in the detector response. Nevertheless, the realization of CG fast neutron spectroscopy has been hindered by the poor discrimination performance of currently available composite scintillators and difficulty in eliminating the effect of chance coincidence events. In this study, CG fast neutron spectroscopy was realized for the first time based on a composite scintillator proposed in our previous work. The results of this study show that this spectroscopy technique has a suitable energy range of approximately 0.4–20&#xa0;MeV. For the ²⁴¹Am-Be source, the number of iterations of the recoil and CG spectrum unfolding using a flat default spectrum were 10,000 and 380, respectively. Using the simulated spectrum as a reference, the <InlineEquation ID="IEq1"> <EquationSource Format="TEX">\(R^2\)</EquationSource> <EquationSource Format="MATHML"><math> <msup> <mi>R</mi> <mn>2</mn> </msup> </math></EquationSource> </InlineEquation> values of the recoil and CG unfolded spectra were found to be 0.939 and 0.975, respectively, above 1&#xa0;MeV. These results indicate that CG fast neutron spectroscopy significantly alleviates the difficulty of spectrum unfolding and exhibits better energy resolution and precision. The technique presented in this work can be applied in neutron metrology laboratories and other nuclear facilities.</p>