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Accordingly, there remains a need for natural-polymer-rich materials (&amp;gt;50% natural content) that can support architected, centimeter-scale scaffolds while integrating molecular-delivery and mineralization functions for volumetric bone engineering. Here, we investigated a hybrid polyelectrolyte complex (PEC) composed of chitosan and polystyrene sulfonate (CS\/PSS) for the development of porous, channeled centimeter-scale scaffolds for bone regeneration. CS:PSS ratios spanning 1:0.5 to 1:2 were systematically evaluated to establish composition\u2013structure\u2013property relationships governing scaffold formation, architecture, mechanical behavior, and biofunctionality. The near-stoichiometric 1:1 formulation was identified as the most balanced composition, combining elastic recovery, mechanical robustness, interconnected porosity, cytocompatibility, self-mineralization, and charge-mediated drug delivery. Sacrificial templating was then used to fabricate volumetric CS\/PSS porous scaffolds (&amp;gt;1 cm3) with defined microchannel networks (200\u2013300 \u03bcm) that maintained structural integrity under dynamic cell seeding and culture while supporting volumetric tissue ingrowth. Leveraging intrinsic electrostatic interactions within the CS\/PSS network, charged molecules, including the osteogenic cue \u03b2-glycerophosphate (\u03b2-GP), were loaded into the scaffold to achieve sustained release governed by hindered diffusion. Notably, scaffold-incorporated \u03b2-GP promoted osteogenic-associated behavior, collagen deposition, and mineral formation comparable to \u03b2-GP supplementation in the culture medium, despite an approximately 10-fold lower cumulative dose. Microcomputed tomography and histological analyses further showed that scaffold-mediated \u03b2-GP localization improved mineral uniformity throughout the scaffold volume relative to media supplementation. Collectively, these findings establish CS\/PSS as a hybrid polyelectrolyte complex platform for integrating structural stability, localized molecular delivery, and architected bone scaffold design, while highlighting strong\/weak polyelectrolyte coupling as a promising strategy for translating natural-polymer-rich systems into robust centimeter-scale scaffolds.<\/jats:p>","DOI":"10.1021\/acsabm.6c00665","type":"journal-article","created":{"date-parts":[[2026,8,7]],"date-time":"2026-08-07T14:01:49Z","timestamp":1786111309000},"page":"8487-8506","source":"Crossref","is-referenced-by-count":0,"title":["A Channeled Chitosan-Based Polyelectrolyte Scaffold Platform for Localized Osteogenic Cue Delivery and Spatial Control of Mineralization in Centimeter-Scale Constructs"],"prefix":"10.1021","volume":"9","author":[{"given":"Rana","family":"Ibrahim","sequence":"first","affiliation":[{"name":"Stevens Institute of Technology , , , ,","place":["Hoboken, New Jersey, United States, 07030"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nicole","family":"Petrocelli","sequence":"additional","affiliation":[{"name":"Stevens Institute of Technology , , , ,","place":["Hoboken, New Jersey, United States, 07030"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Matangi Parimala Chelvi","family":"Ratnamani","sequence":"additional","affiliation":[{"name":"Stevens Institute of Technology , , , ,","place":["Hoboken, New Jersey, United States, 07030"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Maya","family":"Lapinski","sequence":"additional","affiliation":[{"name":"Stevens Institute of Technology , , , ,","place":["Hoboken, New Jersey, United States, 07030"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Erfan","family":"Sarhaadei","sequence":"additional","affiliation":[{"name":"Stevens Institute of Technology , , , ,","place":["Hoboken, New Jersey, United States, 07030"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"William","family":"Querido","sequence":"additional","affiliation":[{"name":"Stevens Institute of Technology , , , ,","place":["Hoboken, New Jersey, United States, 07030"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3455-8523","authenticated-orcid":true,"given":"Hongjun","family":"Wang","sequence":"additional","affiliation":[{"name":"Stevens Institute of Technology , , , ,","place":["Hoboken, New Jersey, United States, 07030"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,7]]},"reference":[{"key":"2026092100084054600_cit1","doi-asserted-by":"publisher","first-page":"389","DOI":"10.1089\/ten.teb.2011.0475","article-title":"Bone Tissue Engineering and Regeneration: From Discovery to the Clinic-an Overview","volume":"17","author":"O\u2019Keefe","year":"2011","journal-title":"Tissue Eng., Part B"},{"issue":"3","key":"2026092100084054600_cit2","doi-asserted-by":"publisher","first-page":"718","DOI":"10.1007\/s10439-015-1253-3","article-title":"Vascularization in Bone Tissue Engineering Constructs","volume":"43","author":"Mercado-Pag\u00e1n","year":"2015","journal-title":"Ann. 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