The molecular spatial structure and electronic energy levels of MDF-2 oligoetheracrylate have been theoretically investigated using a Hyperchem 4.5 computer package. We have optimized the MDF-2 geometry, obtaining a non-linear structure with one benzene ring situated near one of the molecule ends. The electron charge density of the MDF-2 photopolymer is distributed non-uniformly, showing the highest absolute values in the vicinity of the benzene ring. C double chemical bonds are perpendicular with regard to the central chain. We have calculated a relatively large value of the HOMO-LUMO energy gap on one hand and, on the other hand, we have estimated a substantially smaller experimental energy gap based on our spectroscopic measurements. An essential influence of the benzene rings on the non-linear optical properties has also been suggested. To check the above semi-empirical results, ab initio calculations have been performed for the molecule fragments as well as for the full MDF-2 structure. An enlarged structure (a tetramer) has also been investigated using the UHF method with a PM3 parametrization.