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The family of adenosylcobalamin(AdoCbl)coenzyme dependent enzymes catalyzes many biologically important reactions; these enzymes are distinguished by the catalysis of carbon skeleton rearrangements(class Ⅰ), heteroatom elimination(class Ⅱ)and Pyridoxal phosphate assisted amine rearrangements(class Ⅲ).In these enzymes, some of the most difficult chemical reactions are carried out by electron deficient free radical species of extreme reactivity.Therefore, EPR, ENDOR, ESEEM, and pulsed-EPR spectroscopy would allow us to identify the radical intermediates participating in the reaction, to measure the radical reaction kinetics, and nanoseconds time resolved changes in the hyperfine and nuclear quadruple interactions.