Here, we introduce a newclass of MTs featuring small-molecule inhibitors as binding motifs.Specifically, we present PARPi-MT, composed of a photocleavableand luminescent Ru­(II)-based reporter and the poly­(ADP-ribose) polymerase(PARP) inhibitor Olaparib for the targeted bimodal imaging of PARP1in H446 xenograft tumor and mouse brain sections, via desorption electrosprayionization (DESI)-MSI and fluorescence microscopy. The gene discussed is PARP1; the disease is neoplasm.