The nuclear magnetic relaxation times in the domain and domain wall of pure natural iron have been measured separately. We have witnessed that the spin-spin relaxation time T-2 is longer than the spin-lattice relaxation time T-1 in the domain wall. The ratio T-2/T-1 increases and approaches 2 with decreasing rf pulse power level. This is due to the anisotropy in the fluctuation of the hyperfine field by single magnon processes or wall-type excitations. The measured spin-spin relaxation rate is well described by the sum of the nonsecular term and the dipole-dipole interaction term.