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Quantum coherence, present whenever a quantum system exists in a superposition of multiple classically distinct states, marks one of the fundamental departures from classical physics. Quantum coherence has recently been investigated rigorously within a resource-theoretic formalism. However, the finer-grained notion of multilevel coherence, which explicitly takes into account the number of superposed classical states, has remained relatively unexplored. A comprehensive analysis of multilevel coherence, which acts as the single-party analogue to multipartite entanglement, is essential for understanding natural quantum processes as well as for gauging the performance of quantum technologies. Here, we develop the theoretical and experimental groundwork for characterizing and quantifying multilevel coherence. We prove that nontrivial levels of purity are required for multilevel coherence, as there is a ball of …