Heavy metals are important sources of environmental pollution and cause disease in organisms throughout the food chain. A localized surface plasmon resonance sensor was proposed and demonstrated to realize Ni2+ detection by using ion-imprinted chitosan. Au nanoparticles were coated on the multimode fiber to excite the local surface plasmon resonance, and Ni2+-imprinted chitosan was then functionalized by using the dip coating technique. Ethylene diamine tetra-acetic acid was used to release the Ni2+ ions and hence form countless voids. Ni2+ was refilled into the voids to increase the refractive index of the sensing material, thus realizing the measurement of Ni2+ by monitoring the wavelength shift in the localized surface plasmon resonant peak. The coating thickness of the Ni2+-chitosan gel was optimized to obtain greater sensitivity. Experimental results show that the proposed Ni2+ sensor has a sensitivity of 185 pm/μM, and the limit of detection is 0.512 μM. The comparison experiments indicated that the ion-imprinted chitosan has better selectivity than pure chitosan.