Organic spintronics is a new emerging field that deals with the spin-related phenomena of organic materials under the influence of a magnetic field. However, there remain some challenges in organic spintronics including (i) low conductivity and massive disorders of organic thin films blocking the way to controllable spin transport, (ii) relatively low magnetic-field sensitivity of organic magnetoresistance (OMAR) devices with tangled working mechanisms and short of methods for sensitivity improvement. Here, we report the realization of OMAR devices based on organic single crystals. The lesser amount of impurities and defects in crystals guarantees a reduction in spin and charge scatterings, so that the OMAR devices exhibit both a small Lorentz function fitting parameter B 0 of 2.3 mT and a non-Lorentz function fitting parameter B 1 of 0.86 mT in the strictly limited bipolaron model. Moreover, we demonstrate the effect of aggregation and intrinsic trap states, pointing out a way for the improvement of the sensitivity.