Biomolecule-based coordination complex nanoassemblies are a new type of functional materials that are attracting increasing attention. They could possess functionalities that are not readily attainable with other materials, and represent a promising research area that can be exploited in coordination chemistry and materials science. Using bioactive folic acid molecule as a linker, Ni-folate-hydrazine coordination complex nanotubes (CCNTs) have been effectively constructed using the solvothermal method. This is not only the first example of the CCNTs being formed using a nonpyridyl-based molecule as a linker, but also the first report on biomolecule-based CCNTs (BMB-CCNTs) with anticancer activity. It does not require any post treatment to achieve targeted delivery and biocompatible performance. The BMB-CCNTs are sufficiently stable at normal pH of 7.4 until it enters a tumor cell, subsequently it breaks open to release drug in the tumor cell. Furthermore, it overcomes the major limitations of antibody-drug and folate-drug conjugates and is a potential smart multi-functional nanomedicine system. The results of in vitro cytotoxicity assay reveal that the antitumor ability of BMB-CCNTs is similar to cisplatin (CDDP), while their cytotoxicity for normal cells is lower than the latter. Furthermore, BMB-CCNTs exhibit excellent performance as drug carriers and target agents for delivering drugs into tumor cells. Bio-TEM and confocal laser scanning microscope images trace the uptake process of CDDP-CCNTs by a tumor cell. CDDP-CCNTs exhibit dual anti-cancer effect.