The novel dysprosium borate DyB5O8(OH)2 was synthesized in a Walker‐type multianvil apparatus at a pressure of 2.5 GPa and a temperature of 673 K. Single‐crystal diffraction data provided the basis for the structure solution and refinement. The compound crystallizes in the acentric monoclinic space group C2 (no. 5) with the lattice parameters a = 7.9288(5), b = 4.4009(3), c = 9.3409(8) Å, and a monoclinic angle of 113.76(1)°. Generally, DyB5O8(OH)2 is comprised of a layer‐like structure consisting of corner sharing [BO4]5– tetrahedra forming dreier and sechser rings, and eightfold coordinated dysprosium cations. Further characterizations were performed by IR and luminescence spectroscopy as well as high‐temperature X‐ray diffraction.