The Kochen-Specker theorem shows the incompatibility of noncontextual hidden variable theories with quantum mechanics. Quantum contextuality is a more general concept than quantum non-locality which is quite well tested in experiments using Bell inequalities. Within neutron interferometry we performed an experimental test of the Kochen-Specker theorem with an inequality, which identifies quantum contextuality, by using spin-path entanglement of single neutrons. Here entanglement is achieved not between different particles, but between degrees of freedom of a single neutron, i.e., between spin and path degree of freedom. Appropriate combinations of the spin analysis and the position of the phase shifter allow an experimental verification of the violation of an inequality derived from the Kochen-Specker theorem. The observed violation 2.291±0.008≰1 clearly shows that quantum mechanical predictions cannot be reproduced by noncontextual hidden variable theories.