In the recent decade, marine origin products have been growingly studied as building blocks complying with the
constant demand of the biomedical sector regarding the development of new devices for Tissue Engineering and
Regenerative Medicine (TERM). In this work, several combinations of marine collagen-chitosan-fucoidan
hydrogel were formed using a newly developed eco-friendly compressive and absorption methodology to produce
hydrogels (CAMPH), which consists of compacting the biopolymers solution while removing the excess of
water. The hydrogel formulations were prepared by blending solutions of 5% collagen from jellyfish and/or 3%
collagen from blue shark skin, with solutions of 3% chitosan from squid pens and solutions of 10% fucoidan from
brown algae, at different ratios. The biopolymer physico-chemical characterization comprised Amino Acid
analysis, ATR-FTIR, CD, SDS-PAGE, ICP, XRD, and the results suggested the shark/jellyfish collagen(s) conserved
the triple helical structure and had similarities with type I and type II collagen, respectively. The studied collagens
also contain a denaturation temperature of around 30–32 ◦C and a molecular weight between 120 and
125 kDa. Additionally, the hydrogel properties were determined by rheology, water uptake ability, degradation
rate, and SEM, and the results showed that all formulations had interesting mechanical (strong viscoelastic
character) and structural stability properties, with a significant positive highlight in the formulation of H3
(blending all biopolymers, i.e., 5% collagen from jellyfish, 3% collagen from skin shark, 3% chitosan and 10% of
fucoidan) in the degradation test, that shows a mass loss around 18% over the 30 days, while the H1 and H2,
present a mass loss of around 35% and 44%, respectively. Additionally, the in vitro cellular assessments using
chondrocyte cells (ATDC5) in encapsulated state revealed, for all hydrogel formulations, a non-cytotoxic
behavior. Furthermore, Live/Dead assay and Phalloidin/DAPI staining, to assess the cytoskeletal organization,
proved that the hydrogels can provide a suitable microenvironment for cell adhesion, viability, and proliferation,
after being encapsulated. Overall, the results show that all marine collagen (jellyfish/shark)-chitosan-fucoidan
hydrogel formulations provide a good structural architecture and microenvironment, highlighting the H3
biomaterial due to containing more polymers in their composition, making it suitable for biomedical articular
cartilage therapies.
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