New actinide borates ThB4O8 and UB4O8 were synthesized under high‐pressure, high‐temperature conditions (5.5 GPa/1100 °C for thorium borate, 10.5 GPa/1100 °C for the isotypic uranium borate) in a Walker‐type multianvil apparatus from their corresponding actinide oxide and boron oxide. The crystal structure was determined on basis of single‐crystal X‐ray diffraction data that were collected at room temperature. Both compounds crystallized in the monoclinic space group C2/c (Z=4). Lattice parameters for ThB4O8: a=1611.3(3), b=419.86(8), c=730.6(2) pm; β=114.70(3)°; V=449.0(2) Å3; R1=0.0255, wR2=0.0653 (all data). Lattice parameters for UB4O8: a=1589.7(3), b=422.14(8), c=723.4(2) pm; β=114.13(3)°; V=443.1(2) Å3; R1=0.0227, wR2=0.0372 (all data). The new AnB4O8 (An=Th, U) structure type is constructed from corner‐sharing BO4 tetrahedra, which form layers in the bc plane. One of the four independent oxygen atoms is threefold‐coordinated. The actinide cations are located between the boron–oxygen layers. In addition to Raman spectroscopic investigations, DFT calculations were performed to support the assignment of the vibrational bands.