The rapid development of unconventional oil and gas resources presents challenges for foam flooding for reservoirs with high salinity and high heterogeneity at elevated temperatures. In this study, hydrophilic anionic sulfonate-modified nanoparticles (NPs) exhibited a synergistic effect with a cationic surfactant in stabilizing N2/water foam in the presence of concentrated divalent ions from ambient temperature up to 70 °C. With low concentrations of both the sulfonated NPs (SNPs) and cationic surfactant, the foams remained stable for 4 days at 50 °C and atmospheric pressure, while the surfactant-stabilized foams collapsed completely in 1 day. This stability mechanism of foams by the SNPs and cationic surfactant is described in terms of phase behavior, bulk shear rheology of the aqueous phase, and the dilational modulus of the gas-brine interface. The high surface elastic dilational modulus E' observed upon addition of the SNP provided stability against coarsening according to the Gibbs criteria. The cryo-SEM images also showed the compact bubble structure of foams provided by the SNPs. Consequently, very minor changes in the foam bubble size were observed at 208 bar (3000 psi) and 50 °C for up to 48 h with only 0.1 wt % or 0.3 wt % SNPs and 0.01 wt % Arquad 12-50, indicating excellent foam stability. The ability of the surfactant and NPs to stabilize foams at low concentrations broadens the application of foams in subsurface reservoirs at high temperatures and salinities.