Response surface methodology was used to simultaneously optimize the electrical and mechanical properties of newly developed conducting biofibers made up of kenaf fiber/polyaniline (KF/PANI). The effect of process parameters such as PANI amount (110 wt.%), dopant concentration (525 N), and molar ratio of aniline/oxidant solutions (0.51.5) were studied using Design of Experiment. Both of the responses (electrical conductivity and unit break) obtained a quadratic model. The experimental values were in good agreement compared to the optimized process. The scanning electron microscope images of the optimized sample revealed uniform PANI component on the KF with nanofibrillar features.