The relay feedback approach is an effective approach for real-time process control. However, it requires accurate limit cycle data. This paper proposes a novel relay feedback approach for fractional-order (FO) controller design to regulate the stable process performance. The proposed methodology does not require prior knowledge of the process and assures accurate limit cycle. Accurate limit cycle parameters are first estimated using the proposed relay. Then, the FO controller is designed based on the output of the limit cycle obtained through the proposed relay, phase, and Nyquist stability criteria. Further, the accuracy of the proposed relay is verified analytically through harmonic analysis. Various performance parameters and indices are estimated and compared with recently published techniques to assess the effectiveness. Additionally, disturbance and parametric uncertainty analyses are conducted to examine the disturbance rejection capacity and robustness. The efficacy of the proposed methodology is further validated on a real-time liquid-level control four-tank process.