On compact Riemann surfaces, the Laplacian has a discrete, non-negative spectrum of eigenvalues of finite multiplicity. The spectrum is intrinsically linked to the geometry of the surface. In this work, we consider surfaces of constant negative curvature with a large symmetry group. It is not possible to calculate explicitly the eigenvalues for surfaces in this class, so we combine group theoretic and analytical methods to derive results about the spectrum. In particular, we focus on the Bolza surface and the Klein quartic. These have the highest order symmetry groups among compact Riemann surfaces of genera 2 and 3 respectively. We analyse the irreducible representations of the full isomorphism group of the Bolza surface and prove that the multiplicity of the first positive eigenvalue is 3, building on the work of Jenni, and identify the irreducible representation that corresponds to this eigenspace. This proof relies on a certain conjecture, for which we give substantial numerical evidence and a hopeful method for proving. We go on to show that the second distinct positive eigenvalue has multiplicity 4.