Structures of small organic and coordination compounds may be calculated rather efficiently and accurately with molecular mechanics. Two major, and still largely unsolved, problems of this method are: (i) the environment of the molecules is usually not included, although with a considerable effort this is basically possible; and (ii) it is not possible with certainty to find the global energy minimum with a general method, a problem that is especially annoying for relatively large systems (more than a few hundred conformers), where all minima may not realistically be screened separately. One possibility addressing both problems consists of combining the computation of structures with experimental results related to the output data of molecular mechanics calculations (nuclear coordinates, strain energies and/or vibrational frequencies). Examples of this approach presented and discussed here indicate that relatively accurate solution structures may be obtained via combinations of molecular mechanics calculations with solution spectra or experimentally determined isomer distributions.