Goethite with protuberant lychee morphology has been synthesized that accomplishes C-H activation of N-methylanilines to generate α-aminonitriles; the catalyst takes oxygen from air and uses it as a co-oxidant in the process. This dataset is associated with the following publication: Verma, S., R.B.N. Baig, R. Varma, and M. Nadagouda. Oxidative C-H activation of amines using protuberant lychee-like goethite. Nature Communications. Nature Publishing Group, London, UK, 8: 2024, (2018).