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Silver/silver chloride nanoparticles (Ag/AgClNPs), with a mean size of 48.2 ± 9.5 nm and a zeta potential value of −31.1 ± 1.9 mV, obtained by the <i>Green Chemistry</i> approach from a mixture of nettle and grape extracts, were used as “building blocks” for the “green” development of plasmonic biohybrids containing biomimetic membranes and chitosan. The mechanism of biohybrid formation was elucidated by optical analyses (UV–vis absorption and emission fluorescence, FTIR, XRD, and SAXS) and microscopic techniques (AFM and SEM). The aforementioned novel materials showed a free radical scavenging capacity of 75% and excellent antimicrobial properties against <i>Escherichia coli</i> (IGZ = 45 mm) and <i>Staphylococcus aureus</i> (IGZ = 35 mm). The antiproliferative activity of biohybrids was highlighted by a therapeutic index value of 1.30 for HT-29 cancer cells and 1.77 for HepG2 cancer cells. At concentrations below 102.2 µM, these materials are not hemolytic, so they will not be harmful when found in the bloodstream. In conclusion, hybrid systems based on phyto-Ag/AgClNPs, artificial cell membranes, and chitosan can be considered potential adjuvants in liver and colorectal cancer treatment.