In the framework of a Green's function theory we report the results of our comprehensive study for the localized vibrational modes (LVMs) associated with microscopic clusters involving N, In and Ga in Ga1–xInx(Alx)NyAs1–y alloys. From the force variation correlation with the bond covalency for the closest mass acceptors CAs(a–) and isoelectronic NAs defects in III‐As we have obtained the corrected value of the interaction parameter for Al‐N bond predicting NAs local mode in AlAs (∼510 cm–1) at a higher frequency than that of GaAs:14N (∼471 cm–1). Various impurity complexes NAs‐Ga4; NAs‐InGa(1)‐Ga3 and NAs‐InGa(2)‐Ga2 are identified by comparing the calculated impurity modes with the existing infrared and Raman scattering spectroscopy data. (© 2009 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)