Structure, spin configuration, magnetocrystalline-anisotropy compensation, magnetization, and magnetostriction of TbxHo0.9−xNd0.1(Fe0.8Co0.2)1.93 (0 ≤ x ≤ 0.40) compounds are investigated. A single-phase Laves phase with MgCu2-type structure is synthesized in equilibrium conditions at ambient pressure. The easy magnetization direction (EMD) is observed toward <1 1 1> axis when x ≥ 0.25, accompanied by a rhombohedral distortion with large spontaneous magnetostriction coefficients λ111. The anisotropy compensation can be achieved by evaluating EMD, magnetization and magnetostriction, and the critical point is realized to be around x=0.25. The good magnetoelastic properties, e.g., the low anisotropy at room temperature, high polycrystalline saturation magnetostriction (λS~560 ppm) and large spontaneous magnetostriction coefficient (λ111~850 ppm), are achieved for the Tb0.25Ho0.65Nd0.1(Fe0.8Co0.2)1.93 compound, which may make it a promising magnetostrictive material.