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Abstract: Studies have been focused on the synthesis of N→Ga‐coordinated organogallium selenides and tellurides [L1Ga(μ‐Se)]2 (1), [L2Ga(μ‐Se)]2 (2) and [L1Ga(μ‐Te)]2 (3), respectively, containing either N,C,N‐ or C,N‐chelating ligands L1, 2 (L1 is {2,6‐(Me2NCH2)2C6H3}− and L2 is {2‐(Et2NCH2)‐4,6‐tBu2‐C6H2}−) having Ga/E (E=Se or Te) atoms in 1/1 ratio. To change the Ga/E ratio, an unusual N→Ga‐coordinated organogallium tetraselenide L1Ga(κ2‐Se4) (4) was prepared. An unprecedented complex (L1Ga)2(μ‐Te2)(μ‐Te) (5), as the result of the non‐stability of 3, was also isolated. Compound 2 is a suitable single‐source precursor for the preparation of amorphous GaSe thin films by the spin coating. Moreover, simple heating of an octadecylamine solution of 2 provided, after work up, monoclinic Ga2Se3 crystals with different crystallinity according to conditions used. Therefore, compound 2 may be also used as a source of Ga2Se3 in the low‐temperature doping process of Bi2Se3. [ABSTRACT FROM AUTHOR]