Shear piezoelectricity has been shown to be linearly proportional to the product of polymer crystallinity and orientation. However, investigations concerning the singular and cumulative effects of these parameters are incomplete since these studies relied exclusively on using orientation to alter crystallinity. In this research, polylactic acid (PLA) samples were fabricated by a dual drawing/annealing process to expand the investigation into the relationship between crystallinity, orientation, and shear piezoelectricity. The results of this study show for the first time that PLA shear piezoelectricity possesses a stronger relationship with the product of crystallinity and orientation than either of these parameters individually. However, this research also shows that processing of PLA for shear piezoelectric applications should focus only on achieving large degrees of orientation, which will inherently lead to increases in crystallinity as well. This approach will optimize PLA's shear sensing capabilities while avoiding certain detrimental effects, specifically embrittlement and a reversal of polymer chain orientation, which can occur during annealing. (C) 2011 Wiley Periodicals, Inc.(dagger) J Polym Sci Part B: Polym Phys 49: 1555-1562, 2011