Silk-fibroin-based biomaterials have been widely utilized for a range of biomaterial-related systems. For all these previously reported systems, the β-sheet forming feature of the silk was the key stabilizing element of the final material structure. Herein, we describe a different strategy, based on the engineering of silk-based ionomers that can yield stable colloidal composites or particle suspensions through electrostatic interactions. These silk-based ionomers were obtained by carbodiimide-mediated coupling of silk fibroin with polylysine hydrobromide and polyglutamic acid sodium salts, respectively. Colloidal composites could be obtained by mixing the ionomeric pair at high concentration (i.e., 25% w/v), while combining them at lower concentrations (i.e., 5% w/v) yielded particle suspensions. The assembly of the ionomers was driven by electrostatic interactions, pH-dependent, and reversible. The network assembly appeared to be polarized, with the interacting poly(amino acid) chains clustered to the core of the particles and the silk backbone oriented outward. In agreement with this assembly mode, doxorubicin, a hydrophilic antitumor drug, could be released at a slow rate, in a pH-dependent manner, indicating that the inside of the ionomeric particles was mainly hydrophilic in nature.
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