Layered double hydroxides (LDH) are matrices with interlayer anions that can be exchanged with several types of organic or inorganic anions. Due to the anion-exchange capability, hundreds of new materials have been prepared in the past two decades. Conversely, attempts to intercalate neutral molecules (and increase the range of applications) have been achieved by expanding the interlayer space with long-chain surfactants, thus allowing to exclusively retain highly hydrophobic molecules. This work describes a folate-intercalated LDH structure, where folate pillars are capable of forming both hydrogen bonds and hydrophobic interactions with neutral molecules. Infrared spectroscopy and X-ray diffraction data indicated that imidazole, urea and cyclophosphamide were successfully intercalated. This evidence increases the opportunity to prepare more novel materials with neutral molecules in LDH. The cyclophosphamide-LDH product here obtained represents a remarkable example of an LDH-based vehicle for a non-ionic anti-cancer drug used in current chemotherapies.