The structures of the helical chiral polymer poly(trityl methacrylate), PTrMA. in solid state and in chloroform solution are compared by using vibrational circular dichroism spectroscopy. The differences between the spectra are discussed in detail based on hand assignments and density functional theory calculations. Therefore, VA and VCD spectra of oligomers of PTrMA were calculated. It is shown that in solution as well as in solid state the helical structure is maintained. Furthermore, it was possible to determine the helical screw sense of the dextrorotary enantiomer (+)-PTrMA to be left-handed.