“…Over the past decades, research on molecular spintronics has been booming, and lots of efforts and great progress have been made in the above research directions. ,,,− However, in fact, the development of this field is still at a relatively primary stage; unclear spin-related theories and scarce spintronic materials and devices make this field step into a bottleneck period of difficulty to improve spin-related performances and achieve innovative multifunctionalities. ,, The concrete key scientific problems causing the tough status are focused on the following aspects. First, from the view of MSCs, the correlations between the chemical and physical structures of MSCs and spin relaxation and transport are unclear, leading it difficult to design and select appropriate and highly efficient MSCs for spintronic applications . Second, there still exists some ambiguous perceptions regarding the ferromagnetic (FM)/MSCs interface properties, including their working principles, influence factors, and controllability .…”