Electron spin resonance spectra of a y-irradiated carbamylcholine chloride, H,NCOOCH,CH,N(CH,),Cl, single crystal has been investigated at room temperature, and the spectra were found to be independent of temperature down to 130 K. The radical was proved to be -CHCH,-, and the g factor and the hyperfine coupling constant of P-protons were found to be isotropic, with the values of 2.0029 and 27.6 G, respectively. The principal values of the hyperfine tensor of the a-proton were found to be A,, = 12.0 G, A,, = 27.6 G and A,, = 3.9 G. The results were found to be in agreement with the a-and P-proton coupling and are discussed.