Materials with different combinations of piezoelectric and flexoelectric properties offer multifunctionality and versatility in terms of modes of operation in sensing, actuation, and energy harvesting. We explore a microscopic mechanism for tailoring the macroscopic quasi-static mechanoelectrical output of polymer-particle composites by taking advantage of heterogeneity-induced enhancement of the stress fields and strain gradient fields. The idea focuses on using microscopic inclusions, such as embedded particles and voids, to manipulate the activation and relative contributions of the piezoelectric and flexoelectric effects under different modes of mechanical excitation, such as uniaxial compression and flexural bending. The material system studied is a composite of poly(vinylidene fluoride-co-trifluoroethylene [P(VDF-TrFE)] polymer and nanoaluminum (nAl) particles, or P(VDF-TrFE)/nAl. This system is interesting because P(VDF-TrFE) exhibits both piezoelectric and flexoelectric behaviors and nAl particles have significantly higher elastic stiffness than the polymer. A range of piezoelectric and flexoelectric properties of P(VDF-TrFE) and the stiffness of the particles are considered. Significant microstructural effects are found to enable tailoring of the mechanoelectrical response through microstructure variation. The responses of the composite are quantified using the effective piezoelectric constant (d33,effo) and the effective flexoelectric coefficient (μTR,effo). It is found that the effective macroscopic piezoelectric and flexoelectric behaviors can be changed either independently or simultaneously through different combinations of microstructure attribute changes. The mechanism revealed points out avenues for developing materials with tunable mechanoelectrical behaviors and multifunctionality.