Commercially available organoclay (Closite 30B) was modified by using 3-aminopropyltriethoxysilane (APS) via a silylation reaction. Sodium clay (Closite Na) was treated by APS directly as a control. Such modified clays were further melt-compounded with polybutylene terephthalate (PBT). The morphology and properties of the modified organoclays were characterized with X-ray diffraction (XRD), transmission electrical microscopy (TEM), Infra-red spectroscopy, contact angle measurement, and thermogravimetric analysis (TGA). The effects of modified clays on the crystallization behavior of PBT were characterized by differential scanning calorimetry. The basal spacing of Closite Na was enlarged from 1.01 to 1.41 nm after APS treatment, indicating that the APS was intercalated into the clay intergalleries as a monolayer. The basal spacing of Closite 30B increased slightly after APS treatment, partially resulted from the reactions between the APS and hydroxyl groups on the intercalant of Closite 30B. Closite 30B was found to be exfoliated disorderly after melt-compounded with PBT. The APS-modified Closite 30B only dispersed as swollen elliptical clay aggregates, in which the silicate layers were orderly intercalated. TGA results showed that the decomposition temperature at 5% weight loss of Closite 30B was increased from 250 to 2708C after APS treatment. A significant increase in the degree of crystallinity of PBT was observed in the exfoliated PBT/30B composite.