Abstract: It has been demonstrated that almost all polymer-clay nanocomposites show higher temperature stability than that of pure polymer, which is attributed to the active exfoliated clay nanosheet firmly adsorbed onto the polymer chains, due to polerization and nucleation effect, the clay nanosheets could protect the polymer chains from destroying. To prove such mechanism, the water-soluble polymer nanocomposites (AAA/SLS-MMT) were synthesized by the in-situ polymerization of 2-acrylamide-2-methyl-propane sulfonic acid, acrylamide, 4-acryloylmorpholine, and organically modified montmorillonite. The techniques of nuclear magnetic resonance, atomic force microscopy and scanning electron microscopy etc., clearly characterized the successful synthesized of sample’s structure, the exfoliated MMT nanosheet adsorbed polymer chain’s scale, and well-dispersed morphology, espectively. The adsorption model, X-ray photoelectron spectroscopy presented the existence of strong adsorption, while molecular simulation calculations first concluded that the strong adsorption energy was −13032.06 kcal/mol. Thermo-gravimetric-analysis proved the temperature of maximum thermal degradation of powder sample (AAA/1.0 wt% SLS-MMT) was over 298 °C. After ageing at 180 °C for 4 h, the apparent viscosity of 5 g/L AAA/1.0 wt% SLS-MMT aqueous solution was 326.7 mPa⋅s, while that of pure polymer (AAA) was only 8.3 mPa⋅s. This optimized sample has the smallest FLAPI value at all test temperatures from 180 to 220 °C in both fresh and salt water based drilling fluid. All the evidences of high temperature resistance indicate that the strong adsorption can enhance the thickness of hydrated shell and adsorption of clay particles in drilling fluid at high temperature. Such mechanism supplied the better way to design high-temperature resistant fluid loss additives for deep and ultra-deep oil and gas formation engineering.