The fluid synergy between experimentalists and theoreticians for decades has led to a deeper understanding of the processes that govern single-molecule magnets. This approach has allowed for the establishment of proven design criteria for the control of magnetic properties through molecular design, the development of new magnetic measurement techniques and innovative computational methodologies. Herein, we give an account of the experimental and theoretical joint endeavor carried out as part of the synthesis group led by David Mills and the computational/theoretical team led by Nicholas Chilton, together with colleagues in synthetic f-element chemistry and magnetism at The University of Manchester. Alongside, we provide a personal perspective on collaborative work in molecular magnetism and how such collaborations are essential for advancing the field further.