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While biofabrication approaches, such as extrusion\u2010based, allow replicating robust, biomimetic, and layered designs, constructs are usually hindered by inadequate phase\/layer integration, poor filler dispersion, and mismatched rheological and mechanical performances. This study introduces an ink engineering strategy as a solution for integrating natural\u2010based nanocomposites in multi\u2010tissue regenerative approaches. For that, two photocrosslinkable natural matrices: a protein\u2013bovine serum albumin methacrylate (BSAMA), and a polysaccharide\u2013hyaluronic acid methacrylate (HAMA)\u2013are selected for their complementary mechanical and cytocompatibility profiles. Bioactive glass nanoparticles, known for osteoconductive potential, are functionalized and covalently immobilized within both matrices through EDC\/NHS chemical coupling. This primary crosslinking enables uniform distribution of inorganic phases, unlocking tuneable rheological properties, adequate for extrusion 3D printing. Then, a secondary crosslinking, leveraging the photo\u2010responsive moieties for post\u2010printing photocuring, enables the obtention of seamlessly integrated robust multi\u2010material constructs. Overall, BSAMA\u2010based inks offer higher cytocompatibility, while HAMA\u2010based inks provide superior mechanical strength. Their combination in multi\u2010material constructs supports hASCs\u2019 metabolic activity and proliferation, confirming bioactivity and cytocompatibility; and finite element modeling validates their mechanical performance, supporting clinical potential for multi\u2010tissue regeneration.<\/jats:p>","DOI":"10.1002\/adhm.202502733","type":"journal-article","created":{"date-parts":[[2025,9,6]],"date-time":"2025-09-06T11:39:41Z","timestamp":1757158781000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Natural\u2010Based Nanocomposite Ink Engineering for Seamless Multi\u2010Material Integration in Extrusion\u2010Based 3D Printing"],"prefix":"10.1002","volume":"15","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1103-6282","authenticated-orcid":false,"given":"Jo\u00e3o R.","family":"Maia","sequence":"first","affiliation":[{"name":"Department of Chemistry CICECO \u2013 Aveiro Institute of Materials University of Aveiro  Aveiro 3810\u2010193 Portugal"}]},{"given":"Miguel","family":"Bilo","sequence":"additional","affiliation":[{"name":"Department of Chemistry CICECO \u2013 Aveiro Institute of Materials University of Aveiro  Aveiro 3810\u2010193 Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7679-8966","authenticated-orcid":false,"given":"Daniel S.","family":"Fidalgo","sequence":"additional","affiliation":[{"name":"Institute of Science and Innovation in Mechanical and Industrial Engineering (INEGI)  R. 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