The spectra of signed matrices have played a fundamental role in social sciences, graph theory, and control theory. In this work, we investigate the computational problems of identifying symmetric signings of matrices with natural spectral properties. Our results are twofold: 1. We show NP-completeness for the following three problems: verifying whether a given matrix has a symmetric signing that is positive semi-definite/singular/has bounded eigenvalues. However, we also illustrate that the complexity could substantially differ for input matrices that are adjacency matrices of graphs. 2. We exhibit a stark contrast between invertibility and the above-mentioned spectral properties: we show a combinatorial characterization of matrices with invertible symmetric signings and design an efficient algorithm using this characterization to verify whether a given matrix has an invertible symmetric signing. Next, we give an efficient algorithm to solve the search problem of finding an invertible symmetric signing for matrices whose support graph is bipartite. We also provide a lower bound on the number of invertible symmetric signed adjacency matrices. Finally, we give an efficient algorithm to find a minimum increase in support of a given symmetric matrix so that it has an invertible symmetric signing. We use combinatorial and spectral techniques in addition to classic results from matching theory. Our combinatorial characterization of matrices with invertible symmetric signings might be of independent interest.