Previously, some attempts have been made to obtain 2D IR spectra from quantumchemical calculations. Mukamel and coworkers employed a fourth-order Taylor expansion of the potential-energy expansion as basis of an exciton Hamiltonian. Subsequently, second-order vibrational perturbation theory has been applied for modeling 2D IR spectra of metal carbonyls and of deuterated glycolaldehyde. Sibert and co-workers constructed a model of harmonically-coupled Morse oscillators and applied it to model the 2D IR spectra of carbonyl complexes. More recently, Besley and coworkers 82 employed calculations in the harmonic approximation in combination with a localization of normal modes to extract the parameters of an exciton model (local-mode frequencies and harmonic couplings). They then applied an empirical anharmonicity on top of this model to simulate the amide I 2D IR spectra of small peptides. Bowman, Tokmakoff, and coworkers employed high-level VSCF/VCI calculations in combination with a local monomer approximation for protonated water clusters in order to interpret 2D IR spectra. Here, our goal is to devise a computational protocol that is efficient and parameter-free and that allows for both the direct prediction of 2D IR spectra for arbitrary molecular systems and can serve as reference for the parametrization of vibrational maps as needed for empirical exciton models. This work is organized as follows. In Section 2, we review the methodology applied for the quantum-chemical calculation of anharmonic vibrational energy levels and transition dipole moments with L-VSCF and L-VCI (Sections 2.1 and 2.2), discuss the connection to vibrational exciton models (Section 2.3), and recall the theory for the calculation of 2D IR spectra (Section 2.4). In Section 3 we give the details of our computational protocol.