The　polycrystalline　Tb0.27Dy0.73-xNdxFe2　Laves　phase　compounds　were　prepared　at　equilibrium　conditions　and　consequent　annealing　method　at　high　pressure.　Their　structural,　spin　configuration,　magnetic　and　magnetostrictive　properties　were　studied.　Rietveld　refinement　analysis　of　X-ray　diffraction　(XRD)　reveals　that　the　studied　compounds　possess　predominantly　the　MgCu2-type　cubic　Laves　phase,　coexisting　with　a　small　amount　of　hcp-type　rare-earth　(RE)-rich　phase　and　PuNi3-type　REFe3　phase.　The　magnetization　(MS)　and　Curie　temperature　(TC)　decrease　while　the　lattice　parameter　increases　with　the　increase　in　Nd　concentration.　The　direction　of　easy　magnetization　(EMD)　accompanied　by　a　rhombohedral　distortion　(λ111)　was　observed　along　[111]　axis　at　room　temperature　(RT).　The　spin　reorientation　transition　(SRT)　occurs　at　low　temperature,　which　was　explained　by　the　two-sublattice　model.　Based　on　the　experimental　results,　a　detailed　phase　diagram　has　been　designed　for　the　Tb0.27Dy0.73-xNdxFe2　Laves　phase　to　demonstrate　the　different　spin　configurations　and　crystal　structure.　The　anisotropy　compensation　between　the　Nd　and　Dy　sublattices　was　realized　at　x　=　0.1.　The　Nd-containing　Tb0.27Dy0.63Nd0.1Fe2　Laves　phase　compound　shows　large　low-field　polycrystalline　magnetostriction　(λS)　and　large　spontaneous　magnetostriction　coefficient　(λ111~1.7　×　10−3),　which　may　make　it　a　good　magnetostrictive　material.　Our　results　indicate　that　the　substitution　of　Nd　by　Dy　in　Tb0.27Dy0.73Fe2　compounds　is　beneficial　for　the　improvement　of　magnetostrictive　properties.　The　present　study　might　be　useful　to　design　Nd-based　magnetostrictive　materials　for　technological　applications.　©　2020　Elsevier　B.V.