The linear and second-order nonlinear susceptibilities of the urea crystal have been evaluated by applying the supermolecule approach. Calculations performed at the time-dependent Hartree-Fock (TDHF) level using the Austin model (AM1) semiempirical Hamiltonian have first demonstrated the almost additive character of the essential polarizability and first hyperpolarizability components. In fact, the only exception concerns the cc (1) component when stacking urea molecules along the c axis, i.e., the axis of the hydrogen bonds. This behavior has been confirmed by ab initio calculations on small clusters. The macroscopic quantities have then been determined by adopting the multiplicative scheme and by correcting the TDHF/AM1 values for missing electron correlation by means of density functional theory and coupled cluster method. The reliability of the multiplicative scheme was demonstrated for clusters as large as 3a×3b×3c. While the electron correlation correction factors are similar for a single molecule and different small clusters, the global performance of the scheme differs for the linear and nonlinear responses. For the second-order nonlinear susceptibility, our predictions are in good agreement with experiment, while for the linear susceptibility and the associated refractive index, our predictions underestimate the experimental values. The limitations of our approach may be attributed to its inability to account for more subtle cooperative effects, like those associated with a network of hydrogen bonds. Together with other works, the supermolecule calculations confirm that the sign of χabc (2) is negative, contrary to an estimate from band structure calculation.