In this work, the tribological performance of bidirectional jute/carbon fiber reinforced polyester composites was investigated using response surface methodology. The effects of three factors namely fiber weight fraction, load, and sliding velocity on the wear and friction values were examined. The composites were fabricated by using compression molding technique and the dry sliding test was conducted using pin-on-disk machine. The response surface methodology coupled with three factors–three-level Box-Behnken design was employed to examine the interactive effects of process variables on wear loss and coefficient of friction. Moreover, Analysis of Variance technique was used to inspect the statistical significance of the developed model. The outcomes revealed that the wear loss increased with the increase in sliding velocity and load and decreased with the increase in weight volume fraction due to diminishing contact between the polyester matrix and rotating disk. However, the coefficient of friction decreased with the increase in process variables. Furthermore, the morphology of worn-out samples was examined using scanning electron microscopy to understand wear mechanisms.