The cover picture shows a partial view of the crystal structure of Ba[Au2SnS4]. A salient property of this crystal structure is the partial framework composed of AuS2 dumbbells and SnS4 tetrahedra to form chains [(Au2SnS4)2–]∞ propagating in the [100] direction. Within the chains a short Au···Au separation of 2.9538(13) Å is observed, while the interchain Au···Au separation is longer at 3.383 Å. The Ba2+ cations (not depicted here) are eightfold coordinated by S2– anions in a distorted bicapped trigonal prismatic environment BaS8. These polyhedra share all S2– anions thus generating a three‐dimensional network. This connection scheme generates voids along [100] hosting the [(Au2SnS4)2–]∞ chains. The short Au···Au separation (dotted lines) is indicative of a relatively strong aurophilic bonding interaction. When irradiated with UV light, Ba[Au2SnS4] is luminescent at the blue‐green spectral range with emission maximum at approximately 21000 cm–1. More Details can be found in the Article by Christoph Ludwig Teske, Huayna Terraschke, Sebastian Mangelsen, and Wolfgang Bensch on page 1716 ff.