Lanthanide metal-organic frameworks (Ln-MOFs) showing single-molecule magnet (SMM) properties are an ever-growing family of materials where the magnetic properties can be tuned by various interrelated parameters, such as the coordinated solvent, temperature, organic linkers, lanthanide ions and their coordination environment. An overview of the general synthetic methodologies to access MOFs/Ln-MOFs and the peculiarities and parameters to control and/or fine-tune their SMM behavior is herein presented. Additionally, diverse challenging strategies for inducing SMM/SIM behavior in an Ln-MOF are discussed, involving redox activity and chirality. Furthermore, intriguing physical phenomena such as the CISS effect and CPL are also highlighted.