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It is reported that dynamical systems over digraphs have superior performance in terms of system damping and tolerance to time delays if the underlying graph Laplacian has a purely real spectrum. This paper investigates the topological conditions under which digraphs possess real or complex Laplacian spectra. We derive sufficient conditions for digraphs, which possibly contain self-loops and negative-weighted edges, to have real Laplacian spectra. The established conditions generally imply that a real Laplacian spectrum is linked to the absence of the so-called digon sign-asymmetric interactions and non-strong connectivity in any subgraph of the digraph. Then, two classes of digraphs with complex Laplacian spectra are identified, which imply that the occurrence of directed cycles is a major factor to cause complex Laplacian eigenvalues. Moreover, we extend our analysis to multilayer digraphs, where strategies for preserving real/complex spectra from graph interconnection are proposed. Numerical experiments demonstrate that the obtained results can effectively guide the redesign of digraph topologies for a better performance.