We developed and examined the applicability of two multimodal paramagnetic contrast agents for the longitudinal in vivo investigations of the brain projections. The classical dextran based neuroanatomical tracer was conjugated with mono- and bimetal Gd(3+) complexes and an optical reporter. Relaxometric studies of both tracer molecules were performed in vitro followed by in cellulo MR and microscopy investigations. Finally, tracers were injected into the motor cortex of the rat brain; uptake and transporting properties were compared by MRI. The advantage of the multimodal approach was taken and histological studies were performed on the same animals. The histology results confirm the MRI studies demonstrating that the applied tracers labelled anterogradely the regions known for their connections with the motor cortex of the rat brain.