Nonaqueous layered silicate suspensions have a complex rheological behavior due to the presence of a microstructure on multiple length scales, which is sensitive to flow and flow history. In the present work, the flow-induced orientation and anisotropy of the nonequilibrium metastable structures in nonaqueous layered silicate suspensions has been studied using a combination of light scattering, scattering dichroism, and advanced rheometric measurements, including two dimensional small amplitude oscillatory shear (2D-SAOS) flow experiments. The nature of the structures during flow was mainly studied by means of small angle light scattering patterns. Linear dichroism measurements in the vorticity and velocity gradient directions were used to assess the microstructural anisotropy. The changes observed in the vorticity plane developed in the same range of shear rate as the shear-thinning behavior of the suspensions. Scattering dichroism was used to demonstrate that the flow-induced anisotropy was locked in upon cessation of flow. To verify that this also leads to an anisotropy of the rheological properties, the linear viscoelastic moduli were measured using (2D-SAOS) experiments. This new technique proved to be particularly sensitive to the anisotropic nature of the metastable microstructure of organoclay suspensions. Both the flow-induced orientation and larger scale microstructural rearrangements are shown to contribute to the transient rheological response of the nonaqueous layered silicate suspensions. (C) 2009 The Society of Rheology. [DOI: 10.1122/1.3094911]