Multilayer network analysis is a useful approach for studying the structural properties of entities with diverse, multitudinous relations. Classifying the importance of nodes and node-layer tuples is an important aspect in the study of multilayer networks. To do this, it is common to calculate various centrality measures, which allow one to rank nodes and node-layers according to a variety of structural features. We formulate occupation, PageRank, betweenness, and closeness centralities in terms of node-occupation properties of different types of continuous-time classical and quantum random walks on multilayer networks. We apply our framework to a variety of synthetic and real-world multilayer networks, and we identify marked differences between classical and quantum centrality measures. Our computations also give insights into the correlations between certain random-walk and geodesic centralities.