The binary compound Sr(3)In(11) (SrIn(3.667)) was synthesized and structurally characterized by X-ray diffraction experiments. It crystallizes in the orthorhombic La(3)Al(11) structure type (space group Immm, Z = 2; a = 4.9257(6), b = 14.247(2), c = 11.212(2) A). The crystal structure of Sr(3)In(11) bears features of the monoclinic EuIn(4) structure, which is adopted by SrIn(4), and the prominent tetragonal BaAl(4) structure. Sr(3)In(11) is stable until 550 degrees C. At higher temperatures it decomposes peritectically into SrIn(2) and In. Structural stability and bonding properties of Sr(3)In(11) were investigated by first principles calculations and compared to SrIn(4) in the monoclinic EuIn(4) and the tetragonal BaAl(4) structure. All three structures consist of a three-dimensional, polyanionic, network formed by In atoms and Sr cations encapsulated in cages. For the BaAl(4)-type SrIn(4), In-In network bonding is perfectly optimized. In contrast, the networks of EuIn(4)-type SrIn(4) and Sr(3)In(11) appear hypo- and hyperelectronic, respectively. The formation of Sr(3)In(11) with a composition close to 1:4 and the nonexistence of BaAl(4)-type SrIn(4) is explained by a delicate interplay of size and electronic factors governing structural stability in the In-rich part of the Sr-In system.