Hydrogels obtained from natural polymers have received widespread attention for their excellent biocompatible property, nontoxicity, easy gelation, and functionalization. Polysaccharides can regulate the gut microbiota and improve the intestinal microenvironment, thus exerting the healthy effect of intestinal immunity. In an active substance delivery system, the extent and speed of the substance reaching its target are highly dependent on the carrier. Thus, the smart active substance delivery systems are gradually increasing. The smart polysaccharide-hydrogels possess the ability in response to external stimuli through changing their volume phase and structure, which are applied in various fields. Natural polysaccharide-based hydrogels possess excellent characteristics of environmental friendliness, good biocompatibility, and abundant sources. According to the response type, natural polysaccharide-based hydrogels are usually divided into stimulus-responsive hydrogels, including internal response (pH, temperature, enzyme, redox) and external response (light, electricity, magnetism) hydrogels. The delivery system based on polysaccharides can exert their effects in the gastrointestinal tract. At the same time, polysaccharides may also take part in regulating the brain signals through the microbiota-gut-brain axis. Therefore, natural polysaccharide-hydrogels are considered as promising biomaterials, which can be designed as delivery systems for regulating the gut-brain axis. This article reviews the research advance of stimulus-responsive hydrogels, which focus on the types, response characteristics, and applications for polysaccharide-based smart hydrogels as delivery systems.