EPR has traditionally been used in order to obtain structural information on transition metal compounds, with exciting frequencies in the range 9–35 GHz. The recent availability of high magnetic field has prompted the use of higher frequencies. In this contribution the advantages of using High-Field-High-Frequency EPR (HF EPR) experiments are reviewed. After a brief introduction aiming to recall the fundamentals of EPR spectroscopy, a short description of the experimental apparatus needed to perform HF EPR measurements is provided. The remaining sections report selected examples showing how much information can be obtained by HF EPR spectra. They range from individual ions with integer spin to molecular clusters. Particular attention is devoted to the so called Single Molecule Magnets, SMM, i.e. to molecular clusters which show slow relaxation of the magnetization at low temperature. This effect is due to Ising type magnetic anisotropy which has been efficiently monitored through HF EPR spectroscopy.