To meet the increasing global demand for energy, better recovery of crude oil from reservoirs must be achieved using methods that are economical and environmentally benign. Here, we have developed a nanofluid of amphiphilic clay-based Janus nanosheets via a facile and scalable method that provides potential to enhance oil recovery. With the aid of dimethyl sulfoxide (DMSO) intercalation and ultrasonication, kaolinite was exfoliated into nanosheets (KaolNS) before being grafted with 3-methacryloxypropyl-triemethoxysilane (KH570) on the Alumina Octahedral Sheet at 40 and 70 °C to form amphiphilic Janus nanosheets (i.e., KaolKH@40 and KaolKH@70). The amphiphilicity and Janus nature of the KaolKH nanosheets have been well demonstrated, with distinct wettability obtained on two sides of the nanosheets, and the KaolKH@70 was more amphiphilic than the KaolKH@40. Upon preparing Pickering emulsion in a hydrophilic glass tube, the KaolKH@40 preferentially stabilized emulsions, while the KaolNS and KaolKH@70 tended to form an observable and high-strength elastic planar interfacial film at the oil–water interface as well as films climbing along the tube’s surface, which were supposed to be the result of emulsion instability and the strong adherence of Janus nanosheets towards tube’s surface. Subsequently, the KaolKH was grafted with poly(N-Isopropylacrylamide) (PNIPAAm), and the prepared thermo-responsive Janus nanosheets demonstrated a reversible transformation between stable emulsion and the observable interfacial films. Finally, when the samples were subjected to core flooding tests, the nanofluid containing 0.01 wt% KaolKH@40 that formed stable emulsions showed an enhanced oil recovery (EOR) rate of 22.37%, outperforming the other nanofluids that formed observable films (an EOR rate ~13%), showcasing the superiority of Pickering emulsions from interfacial films. This work demonstrates that KH-570-modified amphiphilic clay-based Janus nanosheets have the potential to be used to improve oil recovery, especially when it is able to form stable Pickering emulsions.