This study explores the preparation of lubricating oleo-dispersions using electrospun nanofibrous mats made from low-sulfonate lignin (LSL) and polycaprolactone (PCL). The rheological and tribological properties of the oleo-dispersions were significantly modulated for the first time through the exploration of LSL/PCL ratio and electrospinning conditions such as applied voltage, distance between the tip and collector, flow rate, ambient humidity, and collector configuration. Adequate uniform ultrathin fibers and Small-amplitude oscillatory shear (SAOS) functions of the oleo-dispersions, with storage modulus values ranging from 102 to 105 Pa at 25 °C, were obtained with a flow rate of 0.5 ml h-1, an applied voltage of 15 kV, relative humidity 45% and a static collector. The LSL/PCL ratio directly affected the mechanical properties of the membranes, influencing stiffness and wear resistance. Higher PCL content enhanced membrane stiffness, reflected in increased SAOS values, but also led to higher friction coefficients (from 0.11 to 0.18) and more pronounced wear traces (measured by wear diameter: 440 to 860 μm). These interactions underscore the complex relationship between micro- and/or nano-structures and tribological performance. This study establishes a clear link between electrospinning conditions and the performance of oleo-dispersions, offering a versatile platform for the development of customizable, renewable lubricants. These findings contribute to the advancement of sustainable lubrication technologies, demonstrating the potential of tailor-made oleo-dispersions as alternatives to traditional lubricants.