The organic‐intercalated clay composites have aroused attractable interest due to their tremendous application in industry. As a new type of the layered‐structure material, halloysite nanotubes (HNTs) were employed to explore the intercalation relationship between the interlayer property and intercalating agents, which were more significant for the potential application. For this purpose, this work systematically studied the intercalation behaviours of dimethyl sulphoxide, potassium acetate, N ‐methylformamide, methanol, and acrylamide in the layered‐structure HNTs, respectively. The organics‐intercalated HNT composites were determined by a series of characterisations.