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In natural tissues, toughness is often imparted via the combination of fibrous noncovalent self‐assembly with key covalent bond formation. This controlled combination of supramolecular and covalent interactions remains difficult to engineer, yet can provide a clear strategy for advanced biomaterials. Here, a synthetic supramolecular/covalent strategy is investigated for creating a tough hydrogel that embodies the hierarchical fibrous architecture of the extracellular matrix (ECM). A benzene‐1,3,5‐tricarboxamide (BTA)  hydrogelator is developed with synthetically addressable norbornene handles that self‐assembles to form a  and viscoelastic hydrogel. Inspired by collagen's covalent cross‐linking of fibrils, the mechanical properties are reinforced by covalent intra‐ and interfiber cross‐links. At over 90% water, the hydrogels withstand up to 550% tensile strain, 90% compressive strain, and dissipated energy with recoverable hysteresis. The  hydrogels are shear‐thinning,  can be 3D bioprinted with good shape fidelity, and can be toughened via covalent cross‐linking. These materials enable the bioprinting of human mesenchymal stromal cell (hMSC) spheroids and subsequent differentiation into chondrogenic tissue. Collectively, these findings highlight the power of covalent reinforcement of supramolecular fibers, offering a  strategy for the bottom‐up design of dynamic, yet tough,  hydrogels and bioinks."},"dsDescriptionDate":{"typeName":"dsDescriptionDate","multiple":false,"typeClass":"primitive","value":"2023-07-17"}}]},{"typeName":"subject","multiple":true,"typeClass":"controlledVocabulary","value":["Medicine, Health and Life Sciences"]},{"typeName":"language","multiple":true,"typeClass":"controlledVocabulary","value":["English"]},{"typeName":"depositor","multiple":false,"typeClass":"primitive","value":"Hebels, Dennie"},{"typeName":"dateOfDeposit","multiple":false,"typeClass":"primitive","value":"2023-07-17"}]},"dansDataVaultMetadata":{"displayName":"Data Vault Metadata","name":"dansDataVaultMetadata","fields":[{"typeName":"dansDataversePid","multiple":false,"typeClass":"primitive","value":"doi:10.34894/AFBYVF"},{"typeName":"dansDataversePidVersion","multiple":false,"typeClass":"primitive","value":"1.1"},{"typeName":"dansBagId","multiple":false,"typeClass":"primitive","value":"urn:uuid:f967f60d-9a96-4dfd-ad7d-6a4ee5dcd207"},{"typeName":"dansNbn","multiple":false,"typeClass":"primitive","value":"urn:nbn:nl:ui:13-a5d49f5d-edbc-407a-8720-060bb682a29b"}]}},"files":[{"label":"0.5 mole equiv self-healing-24hrs.avi","restricted":false,"directoryLabel":"Index data collection_2/Self-healing/24 hrs/0.5 mole equiv thiol","version":1,"datasetVersionId":30254,"dataFile":{"id":378823,"persistentId":"","filename":"0.5 mole equiv self-healing-24hrs.avi","contentType":"video/x-msvideo","friendlyType":"AVI Video","filesize":17052654,"storageIdentifier":"surf://store:189abe58314-5bad5a13841a","rootDataFileId":-1,"checksum":{"type":"SHA-1","value":"a25b4f7d76ddfbd44ce008f07e20c9327b02b4ab"},"tabularData":false,"creationDate":"2023-07-31","publicationDate":"2023-08-24","directoryLabel":"Index data collection_2/Self-healing/24 hrs/0.5 mole equiv thiol","lastUpdateTime":"2025-02-18T16:27:28Z","fileAccessRequest":false}},{"label":"0.5mole equiv self-healing 2 hrs.avi","restricted":false,"directoryLabel":"Index data collection_2/Self-healing/2 hrs/0.5 mole equivalent thiol","version":1,"datasetVersionId":30254,"dataFile":{"id":378514,"persistentId":"","filename":"0.5mole equiv self-healing 2 hrs.avi","contentType":"video/x-msvideo","friendlyType":"AVI Video","filesize":7517110,"storageIdentifier":"surf://store:189abe56823-89ef76efff2a","rootDataFileId":-1,"checksum":{"type":"SHA-1","value":"70ae7fcbefca2bb93b5dad4bae933189144e5add"},"tabularData":false,"creationDate":"2023-07-31","publicationDate":"2023-08-24","directoryLabel":"Index data collection_2/Self-healing/2 hrs/0.5 mole equivalent thiol","lastUpdateTime":"2025-02-18T16:27:28Z","fileAccessRequest":false}},{"label":"07135329.JPG","restricted":false,"directoryLabel":"Index data collection_2/Bioprinting_hMSC differentiation/Bioprinting Day 7 - 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