Intraparticle entanglement of individual particles such as neutrons could enable another class of scattering probes that are sensitive to entanglement in quantum systems and materials. In this work, we present experimental results demonstrating quantum contextuality as a result of entanglement between the spin and energy modes (i.e., degrees of freedom) of single neutrons in a beam using a pair of resonant radio-frequency neutron spin flippers in the modulated intensity with zero effort configuration. We verified the mode entanglement by measuring a Clauser-Horne-Shimony-Holt contextuality witness S defined in the spin and energy subsystems, observing a clear breach of the classical bound of |S|≤2, obtaining S=2.40±0.02. These entangled beams could enable alternative approaches for directly probing dynamics and entanglement in quantum materials whose low-energy excitation scales match those of the incident entangled neutron.