The phyto-development of nanomaterials is one of the main challenges for scientists today, as it offers unusual properties and multifunctionality. The originality of our paper lies in the study of new materials based on biomimicking lipid bilayers loaded with chlorophyll, chitosan, and turmeric-generated nano-silver/silver chloride particles. These materials showed a good free radical scavenging capacity between 76.25 and 93.26% (in vitro tested through chemiluminescence method) and a good antimicrobial activity against Enterococcus faecalis bacterium (IZ > 10 mm). The anticancer activity of our developed bio-based materials was investigated against two cancer cell lines (human colorectal adenocarcinoma cells HT-29, and human liver carcinoma cells HepG2) and compared to one healthy cell line (human fibroblast BJ cell line). Cell viability was evaluated for all prepared materials after a 24 h treatment and was used to select the biohybrid with the highest therapeutic index (TI); additionally, the hemolytic activity of the samples was also evaluated. Finally, we investigated the morphological changes induced by the developed materials against the cell lines studied. Biophysical studies on these materials were done by correlating UV–Vis and FTIR absorption spectroscopy, with XRD, SANS, and SAXS methods, and with information provided by microscopic techniques (AFM, SEM/EDS). In conclusion, these “green” developed hybrid systems are an important alternative in cancer treatment, and against health problems associated with drug-resistant infections.