Polyurethane/attapulgite (PU/ATT) nanocomposites derived from castor oil were prepared by incorporation of 8 wt % ATT, acid-treated ATT, and KH560-treated ATT. The effects of three ATTs (ATT, acid-ATT, and KH560-ATT) on the comprehensive properties of PU/ATT nanocomposites were systematically investigated. The results showed that the incorporation of 8 wt % of three ATTs could produce an obvious reinforcement on the castor oil-based PU and that the silane modification treatment, rather than the acid treatment, has the more effective reinforcement effect. SEM images revealed the uniform dispersion of ATT in the PU matrix. DMA confirmed that the storage modulus and glass transition temperature (T_g) of PU/ATT nanocomposites were significantly increased after blending with different ATTs. For PU/KH560-ATT8 nanocomposites, the thermal stability of the PU was obviously enhanced by the addition of KH560-ATT. In particular, 8 wt % KH560-ATT loaded castor oil-based PU nanocomposites exhibit an obvious improvement in tensile strength (255%), Young’s modulus (200%), T_g (5.1 °C), the storage modulus at 25 °C (104%), and the initial decomposition temperature (7.7 °C). The prepared bio-based PU materials could be a potential candidate to replace petroleum-based PU products in practical applications.