Poly(vinylidenefluoride) with enhanced electroactive properties is of great interest in energy harvesting and sensing applications. This study aims to elucidate the effects of processing parameters in extrusion, using a desktop extruder or a microcompounder, on the polymorphism of the fabricated poly(vinylidenefluoride) filaments. All samples were characterized by differential scanning calorimetry, Fourier‐transform infrared spectroscopy, and electromechanical testing. Statistical analyses were conducted to correlate the processing parameters with the poly(vinylidenefluoride) filaments' crystal structures. Experimental results revealed that the optimal extrusion temperature at 220°C and stretching ratio of 4.5 to 6.5 would yield poly(vinylidenefluoride) filaments with a degree of crystallinity of up to 58% of which 80% is β‐phase crystals. The finding of this manuscript has the potential to promote the use of poly(vinylidenefluoride) filaments in the fused filament fabrication.