A large amount of waste slurry is generated during construction, but direct sedimentation and transportation increase construction costs. Improper treatment leads to ecological and environmental pollution. This paper proposes to reuse drilling waste slurry (DWS) as a raw material from a particular project as a grouting material for the real-time capsule grouting technique (RCG) to replace cement grouting material. This not only deals with DWS but also solves the material demand of RCG. An orthogonal experimental design evaluated the performance of the DWS grouting material (DWS-GM). The five levels for the three factors of this experiment were selected, including the fluidity, bleeding rate, initial setting time, and compression strength. A linear model, support vector machines, and neural networks were used to construct regression models, and the effects of different contents of cement, bentonite, and fly ash on the DWS-GM performance were analyzed. The SVM regression model had better performance in describing the laws of fluidity, bleeding rate, and 28-day compressive strength. Furthermore, the optimization model is proposed to obtain the optimal formulation of the DWS-GM under specific constraints. The optimization results show that the optimal formulation of the DWS-GM was 5.6% cement and 6.9% bentonite. The BL, FL, IST, and 28DCS were 1.61%, 21.87 cm, 27.05 h, and 0.22 MPa to meet the functional requirements of the DWS-GM. The above research fully proves the feasibility of the DWS reuse application. We will further reuse DWS to develop other multifunctional material applications in combination with the control needs of RCG technology and technology from other fields.