We report on our multi–pronged approach to understand the structural and electrical properties of an InAl(Ga)N(33nm barrier)/Al(Ga)N(1nm interlayer)/GaN(3μm)/ AlN(100nm)/Al2O3 high electron mobility transistor (HEMT) heterostructure grown by metal organic vapor phase epitaxy (MOVPE). In particular we reveal and discuss the role of unintentional Ga incorporation in the barrier and also in the interlayer. The observation of unintentional Ga incorporation by using energy dispersive X–ray spectroscopy analysis in a scanning transmission electron microscope is supported with results obtained for samples with a range of AlN interlayer thicknesses grown under both the showerhead as well as the horizontal type MOVPE reactors. Poisson–Schrödinger simulations show that for high Ga incorporation in the Al(Ga)N interlayer, an additional triangular well with very small depth may be exhibited in parallel to the main 2–DEG channel. The presence of this additional channel may cause parasitic conduction and severe issues in device characteristics and processing. Producing a HEMT structure with InAlGaN as the barrier and AlGaN as the interlayer with appropriate alloy composition may be a possible route to optimization, as it might be difficult to avoid Ga incorporation while continuously depositing the layers using the MOVPE growth method. Our present work shows the necessity of a multicharacterization approach to correlate structural and electrical properties to understand device structures and their performance.