Abstract: | Unlike extensively studied diradicals linked by π‐conjugated systems, only a few studies have investigated weakly coupled diradicals linked by an sp3 carbon atom. Herein, we prepared pyrrolidin‐1‐oxyl–(nitronyl nitroxide)‐dyad 5 and pyrrolidin‐1‐oxyl–iminonitroxide‐dyad 6 . From the observed temperature dependence of the magnetic susceptibility, 5 and 6 were determined to be in singlet ground states with 2Jintra/kB=?35.2 K and ?13.6 K, respectively. From these results and theoretical calculations of related diradicals, the spin‐polarization model counting the small spin density of the sp3 carbon atom could be used as a spin‐prediction model. |