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The anisotropic paramagnetism and specific heat in Nd2Ti2O7 single crystalsare investigated. Angular dependence of the magnetization and Weisstemperatures show the dominant role of the crystal field effect in themagnetization. By incorporating the results from the diluted samples,contributions to Weiss temperature from exchange interactions and crystal fieldinteractions are isolated. The exchange interactions are found to beferromagnetic, while the crystal field contributes a large negative part to theWeiss temperature, along all three crystallographic directions. The specificheat under magnetic field reveals a two-level Schottky ground state scheme, dueto the Zeeman splitting of the ground state doublet, and the g-factors are thusdetermined. These observations provide solid foundations for furtherinvestigations of Nd2Ti2O7.

Anisotropic paramagnetism of monoclinic Nd2Ti2O7 single crystals