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Chronic wounds are associated with infectious microbial complex communities called biofilms. The management of chronic wound infection is limited by the complexity of selecting an appropriate antimicrobial dressing with antibiofilm activity due to antimicrobial resistance in biofilms. Herein, the in situ developed bacterial cellulose/poly(vinyl alcohol) (BC-PVA) composite is ex situ modified with genipin-crosslinked silk sericin (SS) and azithromycin (AZM) (SSga). The composite is evaluated as a wound dressing material for preventing the development, dispersion, and/or eradication of microbial biofilm. Fourier transform infrared spectroscopy confirms the intermolecular interactions between the components of BC-PVA@SSga scaffolds. The addition of PVA during BC production significantly increases the porosity from 53.5% ± 2.3% to 83.5% ± 2.9%, the pore size from 2.3 ± 1.9 to 16.8 ± 4.5 µm, the fiber diameter from 35.5 ± 10 to 120 ± 27.4 nm, and improves the thermal stability and flexibility. Studies using bacteria and fungi indicate high inhibition and disruption of biofilms upon AZM addition. In vitro biocompatibility analysis confirms the nontoxic nature of BC-PVA@SSga toward HaCaT and NIH3T3 cells, whereas the addition of SS enhances cell proliferation. The developed BC-PVA@SSga accelerates wound healing in the infected mouse model, thus can be a promising wound dressing biomaterial.