Abstract (PhSe) 2 reacts with Br 2, ethylenethiourea and PhTeBr 3, further with I 2, ethylenethiourea and PhTeI 3, to give [PhSe(etu)][PhTeBr 4] ( 1) (Ph = phenyl; etu = ethylenethiourea) and [PhSe(etu)][PhTeI 4] ( 2) in very good yields. The tellurium centers present a distorted octahedral configuration, achieved through dimerization involving secondary, reciprocal Te···X interactions. In both compounds the anionic dimmers are linked through X···X interactions, attaining a one-dimensional, polymeric assembly along the b axis. Cations and anions are linked through short Se···X contacts. In addition to single crystal X-ray data, multinuclear NMR results for 1 and 2 are also presented and discussed.