In an accompanying paper by Lee, Allen, and Schaefer [J. Chem. Phys. 87, 7062 (1987)], an efficient formulation for the analytic evaluation of two-configuration self-consistent-field configuration interaction (TCSCF-CI) energy first derivatives is presented. In this paper the TCSCF-CI gradient method is adapted and applied to singlet excited electronic states of the same symmetry as the ground state. Since single-configuration self-consistent-field configuration interaction (SCF-CI) wave functions are unreliable for such electronic states due to the possibility of variational collapse, the TCSCF-CI method based on excited-state orbitals is the simplest means by which dynamical electron correlation can be incorporated effectively. Geometrical structures, excitation energies, and harmonic vibrational frequencies obtained with double-zeta plus polarization (DZP) and DZP+Rydberg (DZP+R) basis sets are reported for the 2 1A1 states of formaldehyde and ketene. The 2 1A1 state of H2CO is found to have two distinct minima with C2v symmetry: a (π→π*)1 valence minimum with re(C–O)=1.564 Å and T0=8.50 eV, and an (n→3py)1 Rydberg minimum with re(C–O)=1.216 Å and T0=7.93 eV. Some question exists on whether the (n→3py)1 state occurs experimentally at 8.11 or 7.96 eV, but in either case the agreement between theory and experiment is good. The 2 1A1 state of CH2CO is found to have only one C2v minimum with re(C–O) =1.129 Å and re(C–C)=1.403 Å. This state is predominantly Rydberg in character and can be designated (π→3px)1, but evidence is presented which suggests a moderate amount of Rydberg–valence mixing involving the (π→π*)1 ‘‘state.’’ The DZP+R CISD T0=6.94 eV prediction confirms previous assignments of the experimental band at 6.78 eV to the 2 1A1 state.