Herein, we aimed to synthesize and characterize chitosan (CS) and phytic acid (PA, CS–PA) polymers and nanoparticles for preparing materials with dye adsorption and drug delivery properties. Based on changes in the solution pH and the molecular weight and concentration of CS and PA, the CS–PA polymers and nanoparticles were prepared using a simple one-step ionic cross-linking protocol. CS–PA nanospheres formed polymers at high CS and PA concentrations, whereas CS–PA nanoparticles were formed at very low concentrations and under suitable pH conditions. Higher concentrations of the material produced denser polymers with a varied nanosphere size. Nanoparticles with different morphologies and sizes were obtained by changing the experimental conditions. Moreover, the self-aggregation of CS molecules in solution was reduced at low concentrations, allowing the easy formation of nanoparticles with regular morphological characteristics with PA. The nanoparticles exhibited good stability under specific conditions. The materials generated here showed promising application in dye adsorption and drug delivery field. This study provides clues for the construction and application of CS-based materials.