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.