Organic single crystals offer the interesting and unique opportunity to investigate the intrinsic electrical behaviour of organic materials, excluding hopping phenomena due to grain boundaries and structural imperfections. Their structural asymmetry permits also to investigate the correlation between their three-dimensional order and their charge transport characteristics. Here we report on millimeter-sized, solution-grown organic single crystals, based on 4-hydroxycyanobenzene (4HCB), which exhibit three-dimensional anisotropic electrical properties along the three crystallographic axes a, b (constituting the main crystal flat face) and c (the crystal thickness), measured over several different samples. The carrier mobility was determined by means of space charge limited current (SCLC) and air-gap field effect transistors fabricated with 4HCB single crystals and the measured value well correlate with the structural packing anisotropy of the molecular crystal. A differential analysis of SCLC curves allowed to determine the distribution and the concentration of the dominant electrically active density of states within the gap.