In this study, Clitoria ternatea was used to provide a quantifiable method for pH measurement. The researchers proposed a new pH measurement method that involves the use of a KrF excimer laser to perform laser-assisted etching of the crown structure of long-period fiber gratings. Processing of the front surface of the optical fibers through grating resulted in periodically structured optical fibers with a sensor diameter of 55 μm and a period of 660 μm; these structured optical fibers were encapsulated using glass slides. On the front surface of the optical fibers, functional group modification of the fiber surface was conducted and a nanogold coating was applied using the self-assembly method. Additionally, Clitoria ternatea was bonded to the surface of the optical fibers for the measurement of refractive index. In the pH sensing experiment, the average loss sensitivity detected by the sensors with no nanogold self-assembled coating was 0.0635 dB/pH. By contrast, the average resonant wavelength sensitivity of the sensors with a nanogold self-assembled coating under localized surface plasmon resonance was increased to 0.173 nm/pH. Compared with the sensors with no nanogold self-assembled coating, the sensors with this coating had a wavelength drift sensitivity enhanced by a factor of 37.