The polycrystalline form of the compound, Tb5Si3, crystallizing in Mn5Si3-type hexagonal structure, which was earlier believe to order antiferromagnetically below 69 K, has been recently reported by us to exhibit interesting magnetoresistance (MR) anomalies. In order to understand the magnetic anomalies of this compound better, we synthesized single crystals of this compound and subjected them to intense magnetization and MR studies. The results reveal that the magnetic behavior is strongly anisotropic as the easy axis is along a basal plane. There appear to be multiple magnetic features in the close vicinity of 70 K. In addition, there are multiple steps in isothermal magnetization (which could not be resolved in the data for polycrystalline data) for magnetic-field (H) along a basal plane. The sign of MR is positive in the magnetically ordered state, and, interestingly, the magnitude dramatically increases at the initial step for H parallel to basal plane, but decreases at subsequent steps as though the origin of these steps are different. However, for the perpendicular orientation (H || [0 0 0 1]), there is no evidence for any step either in M(H) or in MR(H). These results establish this compound is an interesting magnetic material.
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