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Abstract The covid‐19 pandemic has revealed the need for alternative production approaches with low startup costs like electrospinning for filter needs, the most imperative element of the personal protective equipment (PPE). Current attempts in advancing melt electrospinning deal with developing strategies for fiber diameter attenuation toward sub‐micron scale. Here, the attunement in the spinning‐zone temperature known as ''spin‐line temperature profile'' was utilized as a baseline for fiber diameter reduction. The mechanical performance of the melt‐electrospun linear low‐density polyethylene (LLDPE) fibers is reported to characterize their structural transformation with respect to various spin‐line temperature profiles. With an increase in the spin‐line temperature to above 100°C in the area of cone formation, an increased tensile and yield strength along with fiber diameter reduction by four‐folds was demonstrated. A significant increase in toughness, by almost three times, without compromising the stiffness and Young's modulus was observed. The dynamic mechanical analysis revealed that spinning in high temperatures produces changes in the alpha (α) relaxation, contributing to the significant increase in strain at break. These results are significant because polyolefin fibers are an imperative element of medical textiles and PPE. Therefore, developing a correlation for process‐structure‐properties for emerging production techniques like melt electrospinning becomes critical.