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As-electrospun microfiber mats comprising atactic polystyrene (aPS), a low-cost commodity polymer, have demonstrated beneficial electromechanical properties. However, the variability of the electromechanical properties of fiber mats produced using different electrospinning conditions has not been investigated. Therefore, herein, the direct electromechanical properties of aPS fiber mats produced using different deposition times (<i>t</i>_dep) and electrospinning voltages (<i>V</i>_ES) are investigated. The resulting apparent piezoelectric <i>d</i> constant (<i>d</i>_app) of the fiber mats demonstrates a specific peak value for <i>t</i>_dep as high as ~1600 pC N⁻¹ under 1-kPa pressure application after ~0.2-kPa pre-pressure application, although the <i>d</i>_app of the fiber mats produced with some conditions is nearly zero pC·N⁻¹. Furthermore, the peak position of <i>d</i>_app with <i>t</i>_dep is fundamentally determined with <i>σ</i>_Eff0/<i>Y</i>_D(<i>h</i>-<i>h</i>_pre) [<i>σ</i>_Eff0: effective surface charge density, <i>Y</i>_D(<i>h</i>-<i>h</i>_pre): secant modulus of elasticity]. Charge distribution models for fiber mats with different <i>t</i>_dep are established. The models explain the characteristics of the significant changes in <i>Y</i>_D(<i>h</i>-<i>h</i>_pre) and <i>σ</i>_Eff0 with <i>t</i>_dep. These findings provide significant directions for the production of fiber mats with improved direct electromechanical properties.