Ferromagnetic semiconductors with a high Curie temperature (>300 K) are believed to be suitable for future spintronics devices such as spin-light emitting diodes, spin-field effect transistors, and quantum computers. 1,2 The advantages of these devices include increased processing speed, lower power consumption, and higher information density, compared with conventional devices. 2 The recent recovery of organic semiconductors with magnetically aligned spins is also interesting because they can be synthesized under much less stringent conditions than inorganic semiconductors due to the low-temperature processing and mechanical flexibility. In particular, π-conjugated organic semiconductors such as 8-hydroxy-quinoline aluminum (Alq 3 , inset of Figure 1a) may be very good for transport of spin-polarized carriers because of the long spin diffusion length and giant magnetoresistance. 3 However, the spin injection efficiency was too low to be used in spin devices and the operation temperature was below 300 K, which might be attributed to the formation of insulating complexes at the interface of metal/Alq 3 (i.e., the interface roughness increased, causing suppression of spin injection to Alq 3 layer) and the conductivity mismatch. 4 Here we address this low spin injection efficiency issue for Alq 3 and suggest a solution. First let us note that both problems may be simultaneously solved by using organic-based magnets. Tetracyanoethylene-based organic magnets, for example, have been reported to be ferromagnetic at low and even at room temperatures. 5 Thus we attempted to modify Alq 3 itself and make it magnetic; Alq 3 -based magnets, if they possess ferromagnetism at room temperature, would be an ideal spin injection layer to an original semiconductor Alq 3 .A glass coating with 150 nm of indium-tin oxide (ITO) was used as the starting substrate. The ITO samples (after a general cleaning process) were loaded into a thermal evaporator at 1.0 × 10 -6 Torr, on which Co-doped Alq 3 layers with a thickness of 100 nm were coevaporated of pure Co metal (99.99%) and Alq 3 powders at room temperature. The Co concentrations in Alq 3 were determined to be 5% (Co/Al atomic ratio ) 0.5) and 10% (1) using the thickness ratio of Co and Alq 3 . Ni-doped Alq 3 was also prepared by the same method. For the measurement of magnetic properties, a Ag layer was deposited on the organic layers, playing a role in protecting the organic layers from moisture. Magnetization measurement was carried out using a superconducting quantum interference device magnetometer (MPMSXL, Quantum Design Co., Ltd.). We also employed a variety of measurement techniques utilizing synchrotron radiation, including X-ray absorption spectroscopy (XAS), and X-ray magnetic circular dichroism (XMCD) to elucidate the origin of the ferromagnetism in the compound. Figure 1a shows the magnetic curves for the 5% Co-doped Alq 3 at 10 and 300 K. The hysteresis loop of the sample at 10 K showed clear ferromagnetic behavior with a coercive field of 170 Oe and a magnetic momen...