A totally structure-determined organosilver(I) metal-oganic framework(MOF) of [{Ag_(18)(CF_3COO)_(18)(H_2O)_2}{Ag_4(erlotinib)_4}]_n·7nCH_3OH·3nH_2O(1) was first synthesized by the self-assembly of erlotinib drug ligand and silver salts in the study. 1 formed a NbO-like 3D network, which was built from Ag(I)-erlotinib induced chains and 18-core silver(I) nanoclusters. When 1 was dispersed in methanol solution, it formed derivative nanoparticles(1-NPs) with the average size of 3.81 nm. Silver(Ⅰ) ion is an efficient reactive oxygen species(ROS) evocator, whereas the erlotinib ligand possesses the targeting activity towards tumor cells. Therefore, IC_(50) values of 1-NPs for A549 and MRC-5 cells were respectively 0.97 and 7.28 μM, which were lower than IC_(50) value of erlotinib. It should be noted that the 7.5-fold higher inhibition effect on A549 cells allows 1-NPs to be a potential targeting anticancer drug for curing lung cancer. The study opens a new avenue to design anticancer drugs based on organosilver(I)MOF derivatives that can realize the value-added reactivity by combining clinical drugs with ROS-inductive silver(Ⅰ) ion.