In this paper, we report on a methodology for theoretical prediction and optimization of charge sensitivity for ungated AlGaN/GaN high electron mobility transistorbased ion sensors operated in the reference electrode free configuration. We have performed numerical simulations of device sensitivity, specifically the change in channel electron concentration with the change in surface potential, for different Al mole fractions and AlGaN thicknesses. These results can be used for device optimization, signal analysis, and sensor calibration purposes. To validate the model, six ungated AlGaN/GaN transistor-based devices of different Al mole fractions and AlGaN thicknesses were fabricated. These devices were exposed to KOH solutions with different pH values, and the voltage change at the gate area was indirectly measured as a function of ionic concentration. The gain in conductivity across the measured range of pH values was experimentally extracted for each device and closely matched the sensitivity predicted by simulation.