The present work correlates the direction and spread of the magnetization measured by 57Fe Mössbauer absorption with the magnetoelastic coupling factor k for amorphous field-annealed ribbons of the 2605 Metglas family: 2605Co and 2605SC with k = 0.71 and ≳0.9, respectively. The absorption line intensities measured for different orientations of the ribbons relative to the γ-rays allow us to determine the direction of M relative to the ribbon. In particular, the component of the magnetization in the direction of the annealing field ma is maximum for the same annealing temperatures (360 °C for 2605Co and 400 °C for 2605SC) that induce the maximum coupling coefficient. In both cases the in-plane magnetization is maximum along the direction of the annealing field, and ma is as high as 0.95 for 2605SC, while it is 0.75 for 2605Co, thus indicating that the overall spread of magnetization directions in the sample is quite small for the SC ribbon. This implies that the dependence of k on bias field can be understood in terms of a simple moment-rotation model. In studying the effect of higher annealing temperatures, the Mössbauer spectra also show that, for SC ribbons, surface crystallization is produced near 420 °C followed by bulk crystallization near 440 °C, whereas for CO ribbons, bulk crystallization is first observed at 370 °C. In both cases the correlation between the decrease in k and the onset of either surface on bulk crystallization is clear. In addition to the previous results on k, a direct determination of (1−k2) is independently performed by using frequency-dependent ac susceptibility measurements in the range between 1 kHz (constant stress regime) and 1 MHz (near constant strain regime). Although the high-frequency side of the data requires accurate corrections for Eddy-current losses, the kCo and kSC values so far determined are 0.7 and 0.92, respectively. a)Metglas is a registered trademark of the Allied Chemical Corporation. b)Associated with American University. c)Associated with Naval Surface Weapons Center. 1C. Modzelewski, H. Savage, L. Kabacoff, and A. Clark, IEEE Trans. Magn., MAG−17, 2837 (1981).