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Abstract: We report the high frequency electron paramagnetic resonance (HF-EPR) study of Cr3(dpa)4Cl2, a linear tri-atomic (Cr II ) 3 chain, that was reported to be EPR silent at the X-band (9.5GHz). Higher frequencies yield well resolved spectra for this S =2 system even at room temperature. At 30K, our variable frequency (34–400GHz) EPR spectra yield a large axial zero-field splitting (D) of −1.643(1)cm−1 as well as a small rhombic ZFS parameter E =0.0339(4)cm−1; with gx =1.9978(4), gy =1.9972(4), and gz =1.9808(4). The magnetic susceptibility measurements fully support the earlier magnetic susceptibility studies and the current EPR results. The observation of the EPR spectrum of only the S =2 state at room temperature suggests that the ground state is well isolated from the excited states. [Copyright &y& Elsevier]