Summary: The problem of computing spectra of operators is arguably one of the most investigated areas of computational mathematics. However, the problem of computing spectra of general bounded infinite matrices has only recently been solved. We establish some of the foundations of computational spectral theory through the Solvability Complexity Index (SCI) hierarchy, an approach closely related to Smale’s program on the foundations of computational mathematics and McMullen’s results on polynomial root finding with rational maps. Infinite-dimensional problems yield an intricate infinite classification theory, determining which spectral problems can be solved and with what types of algorithms. We provide answers to many longstanding open questions on the existence of algorithms. For example, we show that spectra can be computed, with error control, from point sampling operator coefficients for large classes of partial differential operators on unbounded domains. Further results include: computing spectra of (possibly unbounded) operators on graphs and separable Hilbert spaces with error control; determining if the spectrum intersects a compact set; the computational spectral gap problem and computing spectral classifications at the bottom of the spectrum; and computing discrete spectra, multiplicities, eigenspaces and determining if the discrete spectrum is non-empty. Moreover, the positive results with error control can be used in computer-assisted proofs. In contrast, the negative results preclude computer-assisted proofs for classes of operators as a whole. Our proofs are constructive, yielding a library of new algorithms and techniques that handle problems that before were out of reach. We demonstrate these algorithms on challenging problems, giving concrete examples of the failure of traditional approaches (e.g., “spectral pollution”) compared to the introduced techniques.