A sensitive ammonia sensor based on long-period fiber grating (LPFG) is designed and manufactured for the detection of ammonia concentration in water. Femtosecond laser direct writing technology is used to write LPFGs on standard single-mode silica fiber. A thin layer doped with basic dyes is coated on the optical fiber for sensing by using the sol-gel method. The thicknesses of sol-gel layers, which play a key role in the sensitivity of the LPFG sensor, were carefully studied. Experimental results show that LPFG with a functional layer of ∼340 nm has the best sensing performance, and the detection limit is 0.08 ppm. The response time of the sensor is less than one minute, and the sensor has good repeatability with a short recovery time. Compared with other organic molecules and ions in water, the proposed LPFG sensor has not only good reusability, but also selectivity for the detection of ammonia.