Polymer waste drilling fluid has extremely high stability, and it is difficult to separate solid from liquid, which has become a key bottleneck problem restricting its resource recycling. This study aims to reveal the stability mechanism of polymer waste drilling fluid and explore the destabilization effect and mechanism of ultrasonic waste drilling fluid. Surface analysis techniques such as X-ray energy spectrum and infrared spectrum were used in combination with colloidal chemical methods to study the spatial molecular structure, stability mechanism, and ultrasonic destabilization mechanism of drilling fluid. The results show that the particles in the drilling fluid exist in two forms: uncoated particles and particles coated by polymers, forming a high molecular stable particle system. Among them, rock particles not coated by polymer follow the vacancy stability and Derjaguin-Landau-Verwey-Overbeek (DLVO) stability mechanism, and the weighting material coated by the polymer surface follows the space stability and DLVO stability mechanism. The results of ultrasonic destabilization experiments show that after ultrasonic treatment at 1000 W power for 5 min, coupled with the addition of 0.02% cationic polyacrylamide, the dehydration rate is as high as 81.0%, and the moisture content of the mud cake is as low as 29.3%, achieving an excellent solid-liquid separation effect. Ultrasound destabilizes polymer waste drilling fluid by destroying the long-chain structure of the polymer. This study provides theoretical support and research direction for the research and development of polymer waste drilling fluid destabilization technology.