An electron microscope study was made of the formation and structure of the inner ligament of Mytilus edulis and Pinctada radiata. This part of the ligament is derived from the isthmus cells which are irregular columnar in shape. They exhibit a prominent rough endoplasmic reticulum and a Golgi apparatus, which are concerned with the elaboration of vesicles and granules eventually incorporated into an integral part of the conchiolin. The crystals arise at the calcification front at the inner surface of the ligament and are enclosed in envelopes. They consist of long, needle-shaped, single aragonite crystals widely dispersed in the ligament. Although the components of the shell and ligament are similar, differences between them consist of an increased amount of conchiolin, as well as a decrease in the amount, diversity of form, arrangement and growth of the crystals; all probably related to the specialized function of the ligament. © 1969 Springer-Verlag.