The specific recognition of AT-rich DNA sequences opens up the door to promising diagnostic and/or therapeutic strategies against gene-related diseases. Here, we demonstrate that amphiphilic Pt complexes of the type [Pt(dmba)(N∧N)]NO (dmba = ,-dimethylbenzylamine-κ κ; N∧N = dpq (), dppz (), and dppn ()) recognize AT-rich oligonucleotides over other types of DNA, RNA, and model proteins. The crystal structure of shows the presence of significant π-stacking interactions and a distorted coordination sphere of the d Pt atom. Complex , containing the largest π-conjugated ligand, forms supramolecular assemblies at high concentrations under aqueous environment. However, its aggregation can be promoted in the presence of DNA at concentrations as low as 10 μM in a process that "turns on" its excimer emission around 600 nm. Viscometry, gel electrophoresis, and theoretical calculations demonstrate that binds to minor groove when self-assembled, while the monomers of and intercalate into the DNA. The complexes also inhibit cancer cell growth with low-micromolar IC values in 2D tissue culture and suppress tumor growth in 3D tumor spheroids with a multicellular resistance (MCR) index comparable to that of cisplatin.