Gadolinium-based contrast agents (GBCAs) are widely used in magnetic resonance imaging (MRI) to improve tissue visualization and lesion detection. Despite their widespread clinical use, conventional GBCAs still face important limitations, including relatively low relaxivity and safety concerns associated with gadolinium release and retention. Therefore, the development of next-generation GBCAs requires molecular designs that improve imaging performance while maintaining high stability and minimizing gadolinium exposure. There are several strategies for improving the performance and safety of GBCAs through molecular design. Imaging performance can be improved by increasing relaxivity through ligand design and introducing functional designs. Ligand structure is also closely related to GBCA safety by influencing the thermodynamic stability and kinetic inertness of gadolinium chelates.