Targeted molecular imaging agents (TMIAs) target cell membrane receptors which are biomarkers for diseases such as cancer, thereby “lighting up” the diseased cells selectively. Dual modal agents combine unique advantages of two different imaging methods and is a growing trend with an unmet need. A versatile modular method is presented for the synthesis of single and dual-modal TMIAs for magnetic resonance imaging (MRI), positron emission tomography (PET) and optical molecular imaging (OMI). The modular method provides targeted probes for PET-OMI, PET-MRI and MRI-OMI. When these bind to the receptor, they can undergo internalization into the cell by endocytosis and thereby accumulate in the cell, causing an amplification of signal. This is illustrated by the binding of a targeting agent fastened through a linker to a dual modal agent that includes a NIR dye for OMI combined with a chelated gadolinium metal for enhanced contrast in MRI. Cover art is by Alexandra McKillop.