The new compound Yb5Ni4Ge10 was obtained as single crystals in high yield from reactions run in liquid indium. Single-crystal X-ray diffraction data showed that it crystallizes in the Sc5Co4Si10 structure type in the tetragonal space group P4/mbm. The structure is a three-dimensional framework of [Ni4Ge10] atoms with voids filled by Yb atoms. The Ni and Ge atoms form pentagons, hexagons, and octagons along the ab one-dimensional plane, which are interconnected along the c axis via Ni–Ge–Ni zigzag chains. Magnetic measurements reveal that Yb5Ni4Ge10 crystals show paramagnetic behavior with a lack of long-range magnetic ordering down to 2 K. The magnetic susceptibility deviates from the Curie–Weiss law below 100 K, presumably because of crystal field effects from Yb3+ ions. In specific heat measurements, the compound exhibits non-Fermi-liquid-like behavior at low temperatures.