In this work, we have studied the effects of extrusion die design, resin molecular structure, and lubricant concentration on the properties of PTFE paste extrudates by performing macroscopic extrusion pressure measurements, Raman spectroscopy, differential scanning calorimetry and mechanical testing on the extrudates. Five resins of different molecular structures were tested. We have found that a balance between fibril quantity and quality (in terms of fibril orientation and continuousness) is necessary to ensure acceptable products, as illustrated through the effects of the operating variables on the extrudate tensile strength. The number of fibrils formed during extrusion can be increased by extruding the paste through a die of larger reduction ratio or by decreasing the lubricant content in the paste, thereby increasing the extrusion pressure. However, excessive pressure will cause fibril breakage. By using a die of larger entrance angle, the extent of fibrillation is also increased, although the quality of the fibrils is somewhat compromised. Increasing the die aspect (L/D) ratio does not increase the extent of fibrillation. However, it increases the degree of fibril orientation and ensures smoother extrudate. Finally, we have found that extrudates obtained using a paste of higher molecular weight are mechanically superior.