The field of molecular magnetism has benefited from the fluid synergy between experimentalists and theoreticians for decades This has led to fundamental understanding of the processes that govern Single Molecule Magnets, allowing for the establishment of clear design criteria to control properties and the development of new synthetic methodologies, sophisticated magnetic measurements and innovative computational techniques. Herein we give an overview on the experimental and theoretical collaborative work we carried out as part of the synthesis group led by David Mills and the computational/theoretical team led by Nicholas Chilton at the University of Manchester. Together with this, we provide a perspective on collaborative work in molecular magnetism and how such collaborations are essential for advancing the field further.