A multifunctional nanoscale platform that is self-assembled from a hydrophobic poly( dl-lactide-coglycolide)(PLGA) core and a hydrophilic paramagnetic-folate-coated PEGylated lipid shell (PFPL; PEG=polyethylene glycol) is designed for simultaneous magnetic resonance imaging (MRI) and targeted therapeutics. The nanocomplex has a well-defined core-shell structure which is studied using confocal laser scanning microscopy (CLSM). The paramagnetic diethylenetriaminepentaacetic acid-gadolinium (DTPA-Gd) chelated to the shell layer exhibits significantly higher spin–lattice relaxivity (r1) than the clinically used small-molecular-weight MRI contrast agent Magnevist®. The PLGA core serves as a nanocontainer to load and release the hydrophobic drugs. From a drug-release study, it is found that the modification of the PLGA core with a polymeric liposome shell can be a useful tool for reducing the drug-release rate. Cellular uptake of folate nanocomplex is found to be higher than that of non-folate-nanocomplex due to the folate-binding effect on the cell membrane. This work indicates that the multifunctional platform with combined characteristics applicable to MRI and drug delivery may have great potential in cancer chemotherapy and diagnosis.