The active and passive piezoelectric response of lead zirconium titanate (PZT)-epoxy particulate composites loaded in shear is studied using analytical models, a finite element model and by experiments. The response is compared to that of the same composites when loaded in simple tension. Analogously to bulk PZT, particulate PZT-polymer composites loaded in shear show higher piezoelectric charge coefficient (d ₁₅) and energy density figure of merit (FOM₁₅) values compared to simple tension (d ₃₃) and (FOM₃₃). This outcome demonstrates the as-yet barely explored potential of piezoelectric particulate composites for optimal strain energy harvesting when activated in shear.