Polypyrrole exhibits actuation under electrochemical doping and undoping of the polymer matrix. Active strain and x-ray diffraction measurements are performed in order to correlate the microscopic and macroscopic structural changes occurring during actuation. Under galvanostatic reduction, the film shows first a linear contraction with oxidation state due to expulsion of small anions. At 50% of the as-grown doping level, the film reverses direction and begins to expand, possibly due to incorporation of the larger cations. X-ray diffraction, however, does not show a linear contraction or expansion in the crystalline portions of the polymer. The polymer crystallites go through a sudden contraction in one dimension of approximately 14%, and otherwise remain constant. The contraction in the polypyrrole crystals occurs at the 50% doping level, and may be correlated with the reversal of macroscopic actuation.