a new discipline. According to many outstanding contributions, [5][6][7][8][9] it has already been proven to be a very important and prospective route to promote the progress in this emerging field by making use of the special merits of molecular semiconductors and spinterface, including mechanically flexibility, [10] abundant photoelectric properties, [11] ferroelectric characteristics, [12] as well as magnetic exchange interaction at the interface. [13] Nowadays, multifunction molecular spintronic devices have gradually attracted attention from various research fields. For instance, spin organic lightemitting diode [11] and molecular spin photovoltaic device, [14] which show brand-new device functions, completely distinguished with the common spintronic device, have been first achieved recently by simply integrating the optical-electrical properties of molecules with spin valve, a prototypical spintronic device. Under the rewarding background of the thriving research on molecular semiconductors and fundamental of spintronic devices in the past decades, the study of multifunctional spintronic devices not only conforms to the development trend but also provides a new opportunity for innovative research in both molecular science and spintronics.Molecular spin valve (MSV), a spintronic device, whereby a molecular semiconductor layer is sandwiched between two ferromagnetic (FM) electrodes (Figure 1a), [8,[15][16][17][18] is considered to be the ideal bed for exploiting multifunctional applications. Herein, recent advances of multifunctional molecular spintronic devices, mostly based on MSV configuration, are systematically reviewed. First, recent studies regarding paralleland interactive-type functional molecular spintronic devices are summarized and classified according to the relationship between the working mechanisms. Subsequently, the latest studies on pure-spin-current-type molecular spintronic devices are discussed. Finally, a short summary and future prospects regarding this field are proposed. Parallel-Type Functional Molecular Spintronic DevicesWhen functional molecular semiconductor or spinterfacial engineering is employed in MSV, novel device functions can be created due to molecular properties or introduced spinterfacial effect. If the novel functions as well as the magnetic The field of spintronics has triggered an enormous revolution in information storage since the first observation of giant magnetoresistance (GMR). Molecular semiconductors are characterized by having very long spin relaxation times up to milliseconds, and are thus widely considered to hold immense potential for spintronic applications. Along with the development of molecular spintronics, it is clear that the study of multipurpose spintronic devices has gradually grown into a new research and development direction. The abundant photoelectric properties of molecular semiconductors and the intriguing functionality of the spinterface, together with novel designs of device structures, have promoted the integration of multiple functions a...

Because of the considerable advantages of functional molecules as well as supramolecules, such as the low cost, light weight, flexibility, and large area preparation via the solution method, molecular electronics has grown into an active and rapidly developing research field over the past few decades. Beyond those well-known advantages, a very long spin relaxation time of π-conjugated molecules, due to the weak spin-orbit coupling, facilitates a pioneering but fast-growing research field, known as molecular spintronics. Recently, a series of sustained progresses have been achieved with various π-conjugated molecular matrixes where spin transport is undoubtedly an important point for the spin physical process and multifunctional applications. Currently, most studies on spin transport are carried out with a molecule-based spin valve, which shows a typical geometry with a thin-film molecular layer sandwiched between two ferromagnetic electrodes. In such a device, the spin transport process has been demonstrated to have a close correlation with spin relaxation time and charge carrier mobility of π-conjugated molecules. In this review, the recent advances of spin transport in these two aspects have been systematically summarized. Particularly, spin transport in π-conjugated molecular materials, considered as promising for spintronics development, have also been highlighted, including molecular single crystal, cocrystal, solid solution as well as other highly ordered supramolecular structures.

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