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We present experimental evidence of the generation of distinct types of genuine multipartite entanglement between three degrees of freedom (spin, energy and path) within single-neutron quantum systems. This is achieved via the development of new spin manipulation apparatuses for neutron interferometry and the entanglement is detected via appropriately designed and optimized nonlinear witnesses. Via the applied criteria we reveal even finer properties of the type of the genuine multipartite entanglement that is produced in the experiment. In a subsequent analysis we show the extraordinarily high fidelity of the generated entangled states, proving the outstanding level of controllability of these systems.