In this study, a composite of laser induced graphene (LIG)/ Polyaniline (PANI) was proposed as a flexible pH potentiometric sensor, with a main interest in the physiological range between 7.4 and 9.5 relate to wound healing. PANI provides an effective sensing and selective layer due to its proton and deprotonation dependency on pH, while LIG is a suitable flexible conductive substrate for electrochemical transduction. LIG electrodes were prepared by polyimide irradiation with a 70 W CO2 laser engraver machine working at 225 mm/s and 15% power. Subsequently, the PANI layer was prepared by electropolymerization with cyclic voltammetry (CV) during either 5 or 10 cycles, resulting in LIG/PANI 5C and LIG/PANI 10C electrodes. In the first stage, the sensitivity towards standardized solutions at pH values of 4, 7, and 10 was evaluated using potentiometry for 50 seconds, resulting in slopes of 58.4 mV/dec and 53 mV/dec for LIG/PANI 5C and LIG/PANI 10C, respectively. Due to its proximity to the ideal Nernstian value and hysteresis width of 3.80 mV after three cycles, LIG/PANI 5C was selected for monitoring solutions prepared with phosphate-buffered saline (PBS) that mimic physiological pH conditions. LIG/PANI 5C demonstrated a sensitivity of −47.91 mV/pH and R2 = 0.99459 in this range. Finally, the analytical performance under LIG/PANI 5C flexion was tested by bending it at 38° during measurement, showing a decreased sensitivity but retaining the long-term capability for detection.