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The ‘normal’ three-coordinate iron–NHC complex [(IPr)Fe(N′′)₂] (N″ = N(SiMe₃)₂) rearranges to its abnormal NHC analogue [(aIPr)Fe(N″)₂] (6) on heating, providing a rare abnormal iron–aNHC complex, and the first such three-coordinate complex. The tert-butyl-substituted complex [(I^tBu)Fe(N″)₂] (4) undergoes a thermal decomposition that has not previously been observed in iron–NHC chemistry, resulting in the bis(imidazole) complex [(^tBuIm)₂Fe(N″)₂] (7). A mechanism that involves consecutive C–H and C–N activation is proposed to account for the formation of 7.