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The crystal structure, magnetization, and spontaneous magnetostriction of Tb1-xNdx(Fe0.9B0.1)(2) alloys have been investigated. X-ray diffraction (XRD) analysis shows that the alloys consist predominantly of the cubic Laves phase with a MgCu2-type structure for x less than or equal to 0.55. Increasing in lattice parameter and decreasing in Curie temperature with increasing x from 0 to 0.55 reveals an increment in the Nd content in the Laves phase. The.(440) XRD line of the Laves phase splits doubly when x less than or equal to 0.7 because of a large spontaneous magnetostriction along its (111) easy magnetization direction. The magnetostriction coefficient lambda(111) decreases significantly with increasing x when 0 < x < 0.55. For x greater than or equal to 0.7, it is difficult to achieve saturation magnetization at room temperature due to increased amount of the Nd2Fe14B-type phase with large magnetocrystalline anisotropy.