An eigenvalue $λ$ of a signed graph $S$ of order $n$ is called a main eigenvalue if its eigenspace is not orthogonal to the all-ones vector $j$. Characterizing signed graphs with exactly $k$ $(1\le k\le n)$ distinct main eigenvalues is a problem in algebraic and graph theory that has been studied since 2020. Du et al. (2024, 2026) characterized a class of signed graphs with exactly two main eigenvalues by analyzing a type of multigraph whose base graph is a tree. In this paper, we extend this study to the case where the associated multigraph has a unicyclic base graph, and we conclude by proposing several open problems.