Abstract: 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.