We report CASPT2 calculations on the electronic excited states of several ureas. For monoureas, we find an electric dipole forbidden n -> pi* transition between 180 and 210 nm, dependent on the geometry and substituents of the urea. We find two intense pi(nb) -> pi* transitions between 150 and 210 nm, which account for the absorptions seen in the experimental spectra. The n' -> pi* and pi(b) -> pi* transitions are at wavelengths below 125 nm, which is below the lower limit of the experimental spectra. Parameter sets modeling the charge densities of the electronic transitions have been derived and permit calculations on larger oligoureas, using the exciton matrix method. For glycouril, a urea dimer, both the CASPT2 method and the matrix method yield similar results. Calculations of the electronic circular dichroism spectrum of an oligourea containing eight urea groups indicate that the experimental spectrum cannot be reproduced without the inclusion of electronic excitations involving the side chains. These calculations are one of the first attempts to understand the relationship between the structure and excited states of this class of macromolecule.