Recently, because of the unique properties of anisotropic and isotropic structures, there are more research studies on anisotropic hydrogels. We prepared a gradient anisotropic carboxymethyl cellulose hydrogel (CMC-Al3+) by directionally diffusing aluminum chloride solution. The orientation of carboxymethyl cellulose (CMC) chains is perpendicular to the direction of aluminum ion diffusion. The degree of cross-linking and orientation gradually decrease along the direction of aluminum ion diffusion. Compared with anisotropic hydrogels prepared by other methods, the hydrogels prepared by directionally diffusing aluminum ion solution have a gradient lamellar structure. Because of the large amount of aluminum ions in CMC-Al3+, the hydrogel shows good sensing performance. CMC-Al3+ is packaged with PVC electrical flame retardant tape to produce a strain sensor used to detect human tiny movements, which can accurately and stably monitor tiny movements. Hydrogel-based strain sensors can be widely used in the fields of human-computer intelligence, human-computer interaction, and wearable devices in the future.