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Smart hydrogels comprising carboxymethyl guar gum and polyvinyl alcohol (CMGG/PVA) were fabricated using tetraethyl orthosilicate as crosslinker. The hydrogels were subjected to nonthermal plasma (NTP) treatment using nitrogen and ammonia mixture. An improvement in surface wettability ensuing from NTP-treatment was evident. Topographical studies revealed surface nanotexturing while the bulk attributes remained undeterred. An insignificant ageing effect was observed upon exposure to air for 20 days which indicated the high stability of the NTP-modified hydrogels. The hydrogels displayed higher swellability in intestinal pH than gastric pH. Appreciable biofilm eradication features against E. coli were observed from the NTP-modified hydrogels. Hemolytic assessment confirmed their compatibility with human blood cells. Release profiles from the hydrogels validated the controlled delivery of anticancer drug chrysin to the intestine. Pristine hydrogels were found to be cytocompatible whereas chrysin-loaded hydrogels displayed a strong inhibitory effect on MCF-7 cells. Additionally, the hydrogels were found to be biodegradable. Thus, N2 and NH3 plasma modified CMGG/PVA hydrogels are potent towards diverse biomedical applications. [ABSTRACT FROM AUTHOR]