In full waveform inversion (FWI), Hessian information of the misfit function is of vital importance for accelerating the convergence of the inversion; however, it usually is not feasible to directly calculate the Hessian matrix and its inverse. Although the limited memory Broyden-Fletcher-Goldfarb-Shanno (L-BFGS) or Hessian-free inexact Newton (HFN) methods are able to use approximate Hessian information, the information they collect is limited. The two methods can be interlaced because they are able to provide Hessian information for each other; however, the performance of the hybrid iterative method is dependent on the effective switch between the two methods. We have designed a new scheme to realize the dynamic switch between the two methods based on the decrease ratio (DR) of the misfit function (objective function), and we propose a modified hybrid iterative optimization method. In the new scheme, we compare the DR of the two methods for a given computational cost, and choose the method with a faster DR. Using these steps, the modified method always implements the most efficient method. The results of Marmousi and overthrust model testings indicate that the convergence with our modified method is significantly faster than that in the L-BFGS method with no loss of inversion quality. Moreover, our modified outperforms the enriched method by a little speedup of the convergence. It also exhibits better efficiency than the HFN method.