The goal of this paper is to review briefly our endeavors to increase the dimensionality of molecular-based bimetallic species. We will successively speak about antiferromagnetically coupled Mn(II) Cu(II) binuclear species, ferrimagnetic chain compounds exhibiting three-dimensional metamagnetic or ferromagnetic behavior, two-dimensional compounds, and finally a three-dimensional compound with a fully interlocked structure. We will also emphasize the importance of the local anisotropy of the spin carriers in the coercivity of the molecular-based magnets.