In this work, synthesis and investigations on chitosan-based hydrogels modified with Aloe vera juice are presented. These materials were synthesized by UV radiation. Investigations involved analysis of chemical structure by FTIR spectroscopy, sorption properties in physiological liquids, strength properties by texture analyzer, surface topography by Atomic Force Microscopy (AFM technique), and in vitro cytotoxicity by MTT test using L929 murine fibroblasts. Particular attention was focused both on determining the impact of the amount and the molecular weight of the crosslinker used for the synthesis as well as on the introduced additive on the properties of hydrogels. It was proven that modified hydrogels exhibited higher swelling ability. Introduced additive affected the tensile strength of hydrogels—modified materials showed 23% higher elongation. The greater amount of the crosslinker used in the synthesis, the more compact the structure, leading to the lower elasticity and lower sorption of hydrogels was reported. Above 95%, murine fibroblasts remained viable after 24 h incubation with hydrogels. It indicates that tested materials did not exhibit cytotoxicity toward these lines. Additionally, materials with Aloe vera juice were characterized by lower surface roughness. Conducted investigations allowed us to state that such modified hydrogels may be considered as useful for biomedical purposes.