Metal-organic frameworks (MOFs) biocompatible systems can host enzymes/bacteria/viruses. Herein we synthesized a series of fatty acid amide hydrolase (FAAH)-decorated UiO-66-NH based on Citrus tangerine leaf extract for drug delivery and biosensor applications. Five chemically manipulated FAAH-like benzamides were localized on the UiO-66-NH surface with physical interactions. Comprehensive cellular and molecular analyses were conducted on HEK-293, HeLa, HepG2, PC12, MCF-7, and HT-29 cell lines (cytotoxicity assessment after 24 and 48 h). MTT results proved above 95 and 50% relative cell viability in the absence and presence of the drug, respectively. A complete targeted drug-releasing capability of nanocarriers was demonstrated after capping with leaf extract from Citrus tangerine, with a stimuli-responsive effect in acidic media. Targeted delivery was complete to the nucleus and cytoplasm of HT-29 cell, but merely to the cytoplasm of HeLa cell lines. Nanocarrier could be targeted for drug delivery to the cytoplasm of the HeLa cell line and to both the nucleus and cytoplasm of HT-29 cell lines. MOF-based nanocarriers proved authentic in vivo towards kidney and liver tissues with targeted cancerous cells efficiently. Besides, FAAH-like molecules revealed optical biosensor potential with high selectivity (even ˂5 nM LOD) towards ssDNA, sgRNA, and Anti-cas9 proteins.