The applicability of step-scan impulse/response FT-IR spectroscopy to the rheo-optical study of polymer films is demonstrated by spectral measurements with isotactic polypropylene. A novel piezoelectrically driven microrheometer is employed to apply repetitive impulses to a polymer sample while time-domain spectra are recorded by step-scan FT-IR spectroscopy, The traditional advantages of Fourier transform spectroscopy are retained while providing a second multiplex advantage for the characterization of the time-dependence of the sample response, Reproducible results, consistent with the frequency-domain literature data and having good signal-to-noise ratio, are obtained. The spectral changes due to molecular reorientation are found to be essentially as fast as the mechanical stretching, also consistent with frequency-domain results. To our knowledge, this is the first reported step-scan FT-IR time-domain rheo-optical measurement. This technique appears to be applicable to a variety of polymer samples, The advantages of time-domain measurements over frequency-domain measurements are briefly discussed.