The structural and the magnetic properties of Gd2Fe16Cr compound are investigated by x-ray diffraction and magnetization measurements. The Gd2Fe16Cr compound has a rhombohedral Th2Zn17-type structure. There exist an anisotropic strong spontaneous magnetostriction and a negative thermal expansion in the magnetic state of Gd2Fe16Cr compound. The average thermal expansion coefficient a = -7.03×10^-6/K in a temperature range of 294-454 K and a = -1.31×10^-5/K in 454-572 K are obtained. The spontaneous magnetostrictive deformation and the Curie temperature are discussed.