We use density functional theory calculations to explore the effects of alloying cubic TiN and VN with transition metals M = Nb, Ta, Mo or W at 50% concentrations. The ternary systems obtained are predicted to be supertough, as they are shown to be harder and significantly more ductile compared with reference binary systems. The primary electronic mechanism of this supertoughening effect is shown in a comprehensive electronic structure analysis of these compounds to be the increased valence electron concentration intrinsic to these ternary systems. Our investigations reveal the complex nature of chemical bonding in these compounds, which ultimately explains the observed selective response to stress. The findings presented in this paper thus offer a design route for the synthesis of supertough transition metal nitride alloys via valence electron concentration tuning.