The complete active space (CAS) SCF method in conjunction with multiconfigurational second-order perturbation theory (CASPT2) has been used to study the electronic spectra of a large number of molecules. The wave functions and the transition properties are computed at the CASSCF level, while dynamic correlation contributions to the excitation energies are obtained through the perturbation treatment. The methods yield energies, which are accurate to at least 0.2 eV, except in a few cases, where the CASSCF reference function does not characterize the electronic state with sufficient accuracy. The applications comprise: the polyenes from ethene to octatetraene (cis- and trans-forms); a number of cyclic pentadienes; norbornadiene; benzene, phenol, phosphabenzene, and the azabenzenes; free base porphin; and the nucleic acid base monomers cytosine, uracil, thymine, and guanine. Finally, the photochemistry of the molecules aminobenzonitrile (ABN) and dimethylaminobenzonitrile (DMABN) has also been studied, in particular the double fluorescence that occurs in DMABN. Taken together these studies comprise large amounts of new spectroscopic data of high accuracy, which either confirm existing assignments of experimental data or lead to new predictions and qualitative as well as quantitative understanding of a large number of electronic spectra. Most studies are restricted to ground state geometries (vertical energies), but in a few cases (octatetraene, ABN, and DMABN) also excited state geometries have been determined, thus yielding 0-0 transition energies and emission spectroscopic data.