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While conventional hydrogels can achieve similar hydration to cartilage tissues, their moduli are substantially inferior. Herein, triple network (TN) hydrogels are prepared to synergistically leverage intra\u2010network electrostatic repulsive and hydrophobic interactions, as well as inter\u2010network electrostatic attractive interactions. They are comprised of an anionic 1<jats:sup>st<\/jats:sup> network, a neutral 2<jats:sup>nd<\/jats:sup> network (capable of hydrophobic associations), and a cationic 3<jats:sup>rd<\/jats:sup> network. Collectively, these interactions act synergistically as effective, yet dynamic crosslinks. By tuning the concentration of the cationic 3<jats:sup>rd<\/jats:sup> network, these TN hydrogels achieve high moduli of \u22481.5 to \u22483.5\u00a0MPa without diminishing cartilage\u2010like water contents (\u224880%), strengths, or toughness values. This unprecedented combination of properties poises these TN hydrogels as cartilage substitutes in applications spanning articulating joints, intervertebral discs (IVDs), trachea, and temporomandibular joint disc (TMJ).<\/jats:p>","DOI":"10.1002\/mabi.202200283","type":"journal-article","created":{"date-parts":[[2022,8,30]],"date-time":"2022-08-30T11:46:36Z","timestamp":1661859996000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Ultra\u2010High Modulus Hydrogels Mimicking Cartilage of the Human Body"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-6167-9243","authenticated-orcid":false,"given":"Connor J.","family":"Demott","sequence":"first","affiliation":[{"name":"Department of Biomedical Engineering Texas A&amp;M University  College Station TX 77843\u20103003 USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"McKenzie R.","family":"Jones","sequence":"additional","affiliation":[{"name":"Department of Biomedical Engineering Texas A&amp;M University  College Station TX 77843\u20103003 USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Caleb D.","family":"Chesney","sequence":"additional","affiliation":[{"name":"Department of Biomedical Engineering Texas A&amp;M University  College Station TX 77843\u20103003 USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Daniel J.","family":"Yeisley","sequence":"additional","affiliation":[{"name":"Department of Biomedical Engineering Rensselaer Polytechnic Institute  Troy NY 12180\u20103590 USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Robert A.","family":"Culibrk","sequence":"additional","affiliation":[{"name":"Department of Biomedical Engineering Rensselaer Polytechnic Institute  Troy NY 12180\u20103590 USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Mariah S.","family":"Hahn","sequence":"additional","affiliation":[{"name":"Department of Biomedical Engineering Rensselaer Polytechnic Institute  Troy NY 12180\u20103590 USA"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5428-0461","authenticated-orcid":false,"given":"Melissa A.","family":"Grunlan","sequence":"additional","affiliation":[{"name":"Department of Biomedical Engineering, Department of Materials Science &amp; Engineering, and Department of Chemistry Texas A&amp;M University  College Station TX 77843\u20103003 USA"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"311","published-online":{"date-parts":[[2022,9,7]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"publisher","DOI":"10.1177\/1941738109350438"},{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1152\/jappl.1992.72.1.219"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1177\/154411130301400207"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jbiomech.2009.12.001"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jmbbm.2017.01.037"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1039\/C6BM00068A"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.msec.2011.10.011"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1016\/S0165-5876(98)00003-2"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1097\/01.brs.0000231761.73859.2c"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1177\/1941738113508917"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1288\/00005537-199508000-00009"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1080\/17476348.2018.1495564"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.7162\/S1809-97772012000200010"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ijporl.2007.01.005"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ijscr.2019.04.009"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1001\/archotol.125.6.650"},{"key":"e_1_2_8_17_1","first-page":"2470","volume":"92","author":"Gomoll A. 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