While eigenvalues of graphs are well studied, spectral analysis of complex unit gain graphs is still in its infancy. This thesis considers gain graphs whose gain groups are gradually less and less restricted, with the ultimate goal of classifying gain graphs that are characterized by their spectra. In such cases, the eigenvalues of a gain graph contain sufficient structural information that it might be uniquely (up to certain equivalence relations) constructed when only given its spectrum. First, the first infinite family of directed graphs that is – up to isomorphism – determined by its Hermitian spectrum is obtained. Since the entries of the Hermitian adjacency matrix are complex units, these objects may be thought of as gain graphs with a restricted gain group. It is shown that directed graphs with the desired property are extremely rare. Thereafter, the perspective is generalized to include signs on the edges. By encoding the various edge-vertex incidence relations with sixth roots of unity, the above perspective can again be taken. With an interesting mix of algebraic and combinatorial techniques, all signed directed graphs with degree at most 4 or least multiplicity at most 3 are determined. Subsequently, these characterizations are used to obtain signed directed graphs that are determined by their spectra. Finally, an extensive discussion of complex unit gain graphs in their most general form is offered. After exploring their various notions of symmetry and many interesting ties to complex geometries, gain graphs with exactly two distinct eigenvalues are classified.